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Heavy Water Reactor Physics Review

This document provides a review of the status of heavy water reactor physics studies. It discusses the various reactor concepts being explored, including pressure tube, boiling heavy water, and pressure vessel designs. It notes that extensive studies are being conducted worldwide on heavy water reactor physics. The document aims to summarize the current status of calculation methods, basic data, experimental work, and analytical correlations in heavy water reactor physics. It focuses on the area of "statics", which involves time-independent phenomena like neutron flux distributions and reactor behavior. The review indicates some areas where further physics studies are still needed.

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136 views93 pages

Heavy Water Reactor Physics Review

This document provides a review of the status of heavy water reactor physics studies. It discusses the various reactor concepts being explored, including pressure tube, boiling heavy water, and pressure vessel designs. It notes that extensive studies are being conducted worldwide on heavy water reactor physics. The document aims to summarize the current status of calculation methods, basic data, experimental work, and analytical correlations in heavy water reactor physics. It focuses on the area of "statics", which involves time-independent phenomena like neutron flux distributions and reactor behavior. The review indicates some areas where further physics studies are still needed.

Uploaded by

pcflorido
Copyright
© Attribution Non-Commercial (BY-NC)
We take content rights seriously. If you suspect this is your content, claim it here.
Available Formats
Download as PDF, TXT or read online on Scribd

AEC RESEARCH-& DEVELOPMENT REPORT . .

'

.. .

UC-80 R e a c t o r Technology Special Distribution

A REVIEW OF H A Y WATER REACTOR PHYSICS EV

V. 0 . U o t i n e n and L. C. Schmid

ERRATA
Page 23 should be numbered 22 Page 22 should be numbered 23

R e a c t o r P h y s i c s Department P h y s i c s and E n g i n e e r i n g D i v i s i o n

May 1968

BATTELLE MEMORIAL INSTITUTE PACIFIC NORTHWEST LABORATORY RICHLAND, WASHINGTON 99352

P r i n t e d i n t h e U n i t e d S t a t e s of America A v a i l a b l e from C l e a r i n g h o u s e f o r F e d e r a l S c i e n t i f i c and T e c h n i c a l I n f o r m a t i o n N a t i o n a l Bureau o f S t a n d a r d s , U.S. Department o f Commerce S p r i n g f i e l d , V i r g i n i a 22151 P r i c e : P r i n t e d Copy $3.00; M i c r o f i c h e $0.65

iii
TABLE OF CONTENTS

BNWL- 1119

P a g e No.

....................................................... ACKNOWLEDGMENTS ...............................................


PREFACE

iv

.................................................. CALCULATION& METHODS DEVELOPMENT ............................. A. HISTORICAL BACKGROUND ......................................


INTRODUCTION B. CELL C&CULAT'ONS DEVELOPMENT

.............................

C.

.......................................... .................................... 2. FOREIGN METHODS BASIC DATA AND METHODS USED I N CELL CALCULATIONS ----------1. CROSS SECTIONS ........................................ 2. SLOWING DOWN TREATMENT I N HEAVY WATER REACTORS -------1.
U.S. METHODS

3,
4.

THE EXPERIMENTAL SCATTERING LAW FOR HEAVY WATER .................................................. SCATTERING KERNELS FOR HEAVY WATER

D.

.................... MACROSCOPIC REACTOR CALCULATIONS .......................... 1. HOMOGENEOUS METHODS .................................. 2. HETEROGENEOUS METHODS .................................

22

37 37

111.

REACTOR DATA AND ANALYTICAL CORRELATIONS A.

...................... UNIFORM LATTICES OF RODS ................................. 1. STATUS OF EXPERIMENTAL STUDIES ......................... 2. STATUS OF ANALYTICAL CORRELATIONS .....................
UNIFORM LATTICES OF CLUSTERS

B.

..............................

IV. V.

......................... 2. STATUS OF ANALYTICAL CORRELATIONS ..................... C. POWER REACTORS ............................................. 1. STATUS OF EXPERIMENTAL WORK ........................... 2. STATUS OF ANALYTICAL CORRELATIONS ...................... SUMMARY AND CONCLUSIONS .......................................
1 .
STATUS OF EXPERIMENTAL STUDIES REFERENCES

....................................................

BNWL- 1119

PREFACE T h i s r e p o r t was p r e p a r e d f o r t h e USAEC Heavy Water R e a c t o r Program O f f i c e . The p u r p o s e o f t h e r e p o r t i s t o review t h e

s t a t u s o f heavy w a t e r r e a c t o r p h y s i c s s t u d i e s , and t o i n d i c a t e a r e a s where f u r t h e r s t u d i e s a r e r e q u i r e d . The c o n t e n t s o f t h i s

r e p o r t s u p p o r t t h e c o n c l u s i o n s and recommendations made i n t h e Mavy Water Program P l a n , BNWL-656 D r a f t , March 1, 1968.

ACKNOWLEDGMENTS

W a p p r e c i a t e t h e d e t a i l e d reviews c o n t r i b u t e d by Alan G. Gibbs e on S c a t t e r i n g Kernels f o r Heavy Water and by 0. K. H a r l i n g on t h e Experimental S c a t t e r i n g Law f o r Heavy Water. W acknowledge a l s o e

c o n t r i b u t i o n s by J. L . C a r t e r , Jr. on Slowing Down Theory and by


B. R, Leonard, Jr. and R. [Link] on t h e S t a t u s of Cross S e c t i o n s .

F i n a l l y , i n c o r p o r a t e d i n t h i s review a r e s e v e r a l comments and s u g g e s t i o n s t h a t were made by J . L. C r a n d a l l and H. C. Honeck of

Savannah River Laboratory through correspondence w i t h p e r s o n n e l of t h e Heavy Water Reactor Program O f f i c e .

A REVIEW OF H A Y WATER REACTOR PHYSICS EV V. 0. Uotinen and L. C.

Schmid

I.

INTRODUCTION Many l a b o r a t o r i e s i n t h e USA and a b r o a d a r e a c t i v e l y engaged i n heavy w a t e r r e a c t o r p h y s i c s s t u d i e s . The e x t e n t of t h e s e s t u d i e s i s

e v i d e n c e d by t h e l a r g e number of p a p e r s on D 0 r e a c t o r p h y s i c s 2 p r e s e n t e d i n r e c e n t y e a r s a t i n t e r n a t i o n a l c o n f e r e n c e s and symposia. World-wide i n t e r e s t i n heavy w a t e r r e a c t o r s i s a l s o e v i d e n c e d by t h e i n c r e a s i n g number of heavy w a t e r r e a c t o r s b e i n g b u i l t around t h e w o r l d each year. Furthermore,
i t i s l i k e l y t h a t i n t h e n e a r f u t u r e i n many

p a r t s of t h e w o r l d t h e u s e of heavy w a t e r r e a c t o r s w i l l i n c r e a s e , mainly b e c a u s e of t h e a d v a n t a g e s of b e i n g a b l e t o u s e n a t u r a l uranium f u e l . The p r e s s u r e t u b e c o n c e p t h a s been e x t e n s i v e l y developed i n Canada and s t u d i e d by F r a n c e , Sweden, Germany, I n d i a , Savannah R i v e r L a b o r a t o r y , and Westinghouse. This r e a c t o r i s w e l l developed, i n h e r e n t l y s t a b l e The 20 M e NPD and 200 M e Douglas P o i n t W W The 500 M e P i c k e r i n g W O t h e r examples a r e t h e

and h a s good n e u t r o n economy.

Candu r e a c t o r s a r e o p e r a t i n g i n Canada now. r e a c t o r s a r e being considered f o r t h e f u t u r e .

50 M e MZFR r e a c t o r i n Germany and t h e p l a n n e d 200 M e RAPP r e a c t o r s i n W W


India. The b o i l i n g H 0 concept h a s b e e n s t u d i e d m a i n l y i n Canada, England, 2 and I t a l y .
I t h a s a lowered D 0 i n v e n t o r y and e f f i c i e n t h e a t removal. 2

It s u f f e r s from p o o r n e u t r o n economy b e c a u s e of t h e H 0 and one o f t h e

main p h y s i c s problems i s i n t h e a r e a of s t a b i l i t y and c o n t r o l .

The

W GW B r i t i s h 90 M e S H R r e a c t o r i s o p e r a t i n g and s t u d i e s a r e b e i n g conducted

W L W f o r a Canadian 250 M e BW r e a c t o r and a n I t a l i a n 34 M e CIRENE p r o t o t y p e .

BNWL- 1119

The p r e s s u r e v e s s e l concept w i t h b o i l i n g D 0 has e x c e l l e n t 2 n e u t r o n economy and a l s o r e q u i r e s c a r e f u l i n v e s t i g a t i o n of t h e s t a b i l i t y and c o n t r o l problems. Norway, and I n d i a . This concept has been s t u d i e d mainly i n Sweden,

The Swedish 200 M e Marviken r e a c t o r has begun operW

a t i o n and t h e Norwegian Halden HBWR has been i n o p e r a t i o n f o r s e v e r a l y e a r s . I n a d d i t i o n t o d a t a from r e s e a r c h programs i n s u p p o r t of s p e c i f i c c o n c e p t s , t h e r e a r e d a t a a v a i l a b l e from g e n e r a l D 0 programs of many 2 o t h e r c o u n t r i e s and of l a b o r a t o r i e s i n t h e United S t a t e s f o r e v a l u a t i o n of methods f o r D 0 r e a c t o r s i n g e n e r a l . 2 Reactor p h y s i c s can b e c a t e g o r i z e d i n t o two g e n e r a l a r e a s . g e n e r a l a r e a , k i n e t i c s , i n v o l v e s time-dependent phenomena. The f i r s t

This i n c l u d e s

t h e o v e r a l l k i n e t i c s and c o n t r o l e v a l u a t i o n s , and through them t h e p h y s i c s a s p e c t s of t h e r e a c t o r s a f e t y a n a l y s i s .


A r e c e n t review of t h e

s t a t u s of k i n e t i c s s t u d i e s f o r heavy w a t e r r e a c t o r s has been p u b l i s h e d . (1) The second g e n e r a l a r e a , s t a t i c s , i n v o l v e s time independent phenomena. S t u d i e s i n t h i s a r e a determine t h e l o c a l n e u t r o n f l u x and

f i s s i o n power d i s t r i b u t i o n s , t h e n e u t r o n economy a s s o c i a t e d w i t h d i f f e r e n t r e a c t o r m a t e r i a l s , and t h e burnup p r o p e r t i e s of t h e f u e l and controls. Also i n c l u d e d i n t h i s a r e a a r e t h e f u l l r e a c t o r e v a l u a t i o n s t o

determine t h e i n t e r a c t i o n s between t h e v a r i o u s l a t t i c e components, t h e o v e r a l l r e a c t o r f l u x and power d i s t r i b u t i o n s , t h e c o n t r o l system e f f e c t s , and t h e o v e r a l l r e a c t o r behavior. I n addition, there a r e the determinations

of t h e o p e r a t i n g c o e f f i c i e n t of r e a c t i v i t y , i n c l u d i n g temperature, d e n s i t y , and a c c i d e n t e f f e c t s . The purpose of t h i s r e p o r t i s t o review t h e s t a t u s of heavy w a t e r r e a c t o r p h y s i c s s t u d i e s which f a l l i n t o t h e broad c a t e g o r y of s t a t i c s .

3 S e v e r a l e x c e l l e n t r e v i e w s of heavy-water presented i n the past.

B W - 1119 N L r e a c t o r physics have been

P a r t i c u l a r a t t e n t i o n s h o u l d b e g i v e n t o t h e IAEA

P a n e l on Heavy Water L a t t i c e s (Vienna 1 9 6 3 ) , (2) t h e Geneva Conference of 1964 ( i n c l u d i n g a p a p e r d e s c r i b i n g l a t t i c e s t u d i e s and c r i t i c a l e x p e r i m e n t s i n t h e U.S.) ( 3 ) and a review a r t i c l e on t h e P h y s i c s o f Heavy Water L a t t i c e s by Honeck and

rand all,'^)

p u b l i s h e d i n 1964.

I n t h i s r e p o r t t h e s e e a r l i e r r e p o r t s a r e t a k e n as t h e s t a r t i n g p o i n t , and some m a j o r r e c e n t developments a r e reviewed i n o r d e r t o a r r i v e a t a r e a s o n a b l e p i c t u r e of t h e c u r r e n t s t a t u s of t h e t e c h n o l o g y of D 0 r e a c t o r .

physics.

On t h e b a s i s o f t h i s review some a r e a s a r e i n d i c a t e d where

f u r t h e r work seems n e c e s s a r y . The development o f c a l c u l a t i o n a l methods i n b o t h t h e U n i t e d S t a t e s and a b r o a d w i l l b e d i s c u s s e d . Then some s p e c i f i c e x p e r i m e n t a l and

a n a l y t i c a l s t u d i e s w i l l be discussed t o i n d i c a t e t h e current s t a t e of t h e a r t of D 0 r e a c t o r p h y s i c s .

11.

CALCULATTONAL METHODS DEVELOPMENT


A.

H i s t o r i c a l Background The t r a d i t i o n a l approach used i n t h e a n a l y t i c a l p r e d i c t i o n of t h e p h y s i c s b e h a v i o r of D 0 r e a c t o r s i s r e f e r r e d t o a s t h e r e c i p e

approach.

A s t h e word r e c i p e i m p l i e s , methods f a l l i n g i n t o t h i s

c a t e g o r y a r e meant t o b e r e l a t i v e l y s i m p l e and r a p i d .

The f o u n d a t i o n

f o r t h e s e r e c i p e s i s t h e c l a s s i c a l d e s c r i p t i o n of t h e n e u t r o n s p e c t r u m
as g i v e n by t h e ~ e s t c o t t ' ~model. )

T h i s model c h a r a c t e r i z e s t h e

n e u t r o n s p e c t r u m as w e l l t h e r m a l i z e d and c o n s i s t i n g of two components, a Maxwellian and a 1 / d i s t r i b u t i o n . ~ B a s i c a l l y , t h e r e c i p e codes

are f i t t e d c a l c u l a t i o n s of t h e f o u r - f a c t o r p a r a m e t e r s
t h e d i f f u s i o n p a r a m e t e r s (D, L

(n ,f

, p , ~ ) and

T, )

b a s e d on s e m i - e m p i r i c a l p r o c e d u r e s ,

Some t y p i c a l r e c i p e s a r e t h e Swedish r e c i p e [Link], ( 6 ) and a more r e c e n t v e r s i o n REBUS, code PLUTHARCO,

('I t h e

Canadian r e c i p e LATREP, (')

t h e Euratom

and t h e codes BSQ, ( l o ) ROCKLAND A , (11) NDC, (12) by Savannah R i v e r , U n i t e d The major

and IDIOT, (13) d e v e l o p e d i n t h e U.S.

N u c l e a r , Wes t i n g h o u s e , and Hanford, r e s p e c t i v e l y .

l i m i t a t i o n o f r e c i p e s , which was r e c o g n i z e d e a r l y i n t h e development of D 0 r e a c t o r p h y s i c s , i s t h a t t h e y h a v e a l i m i t e d r a n g e o f a p p l i 2 cability. Each r e c i p e i s a d j u s t e d t o f i t a c e r t a i n r a n g e o f l a t t i c e s

o f a p a r t i c u l a r d e s i g n , and c a n n o t b e a p p l i e d s u c c e s s f u l l y o u t s i d e t h i s range. An a l t e r n a t i v e t o t h e c l a s s i c a l r e c i p e approach h a s b e e n t h e a d a p t a t i o n o f t h e m u l t i - g r o u p codes d e v e l o p e d f o r d e s i g n i n g H 0 2 reactors. These codes c o n s i d e r t h e n e u t r o n p r o c e s s e s i n t h e l a t t i c e

i n g r e a t d e t a i l , and t h e i r u s e c o n s t i t u t e s a much l e s s e m p i r i c a l and more f u n d a m e n t a l c a l c u l a t i o n a l approach t h a n t h e u s e o f r e c i p e s . An example o f a n e a r l y u s e o f t h i s approach i s t h e a n a l y s i s o f t h e CVTR e x p e r i m e n t s by Westinghouse ( I 4 ) i n t h e e a r l y 1 9 6 0 ' s . The

Wes t i n g h o u s e s t u d i e s u t i l i z e d t h e MUFT ( I 5 ) and PIMG ( I 6 ) computer codes f o r t h e s l o w i n g down c a l c u l a t i o n , w i t h an a u x i l i a r y Monte C a r l o c a l c u l a t i o n w i t h t h e REPLICA ( I 7 ) code t o p r o v i d e s e l f - s h i e l d i n g f a c t o r s f o r MUFT; THERMOS ( I 8 ) f o r t h e t h e r m a l i z a t i o n c a l c u l a t i o n ; and t h e two-dimensional calculation. d i f f u s i o n t h e o r y code PDQ (19)f o r t h e r e a c t o r

T h i s approach o f a d a p t i n g l i g h t w a t e r codes t o heavy

w a t e r l a t t i c e s , l e a d s u r p r i s i n g l y t o f a i r l y good s u c c e s s . The p a n e l r e p o r t ( 2 ) on Heavy Water L a t t i c e s , h e l d i n Vienna i n F e b r u a r y o f 1963, c o n t a i n e d s t a t u s r e p o r t s of t h e D 0 r e a c t o r p h y s i c s 2 e f f o r t s of many n a t i o n s . One o f t h e p o i n t s made a t t h i s p a n e l

m e e t i n g ( 2 0 ) was t h a t t h e r e c i p e - t y p e l i m i t e d a r e a s of a p p l i c a b i l i t y .

codes, w h i l e v e r y u s e f u l , had

I t was p r e d i c t e d t h a t r e c i p e s would

remain a s i m p o r t a n t t o o l s f o r D 0 r e a c t o r d e s i g n e r s , b u t a t t h e same 2 t i m e t h e r e would b e an e v e r - i n c r e a s i n g t r e n d toward v e r y d e t a i l e d calculations. The t r e n d toward more fundamental c a l c u l a t i o n a l methods was i l l u s t r a t e d by t h e Westinghouse CVTR a n a l y s i s , ( I 4 ) and a l s o w i t h t h e u s e o f t h e two B r i t i s h c o d e s , METHUSELAH (21)
a t t h e 1963 P a n e l Meeting.

and THULE, (22) i n t r o d u c e d

Both of t h e s e codes had b e e n developed i n The METHUSELAH

s u p p o r t of t h e Steam G e n e r a t i n g Heavy Water R e a c t o r .

code was meant t o b e a d e s i g n code and was modeled a f t e r a four-group d i f f u s i o n t h e o r y scheme of t h e Bet t i s L a b o r a t o r y of Westinghouse. METHUSELAH, however, i s a five-group scheme, w i t h two o v e r l a p p i n g

t h e r m a l g r o u p s , one c h a r a c t e r i s t i c o f t h e m o d e r a t o r r e g i o n and t h e o t h e r c h a r a c t e r i s t i c of t h e f u e l r e g i o n . The code THULE r e p r e s e n t e d

t h e most e x a c t c a l c u l a t i o n f e a s i b l e a t t h e t i m e , and w a s developed and used t o check t h e v a l i d i t y of METHUSELAH c a l c u l a t i o n s . The THULE

code, which w a s b u i l t around t h e e x i s t i n g multi-group C a r l s o n T r a n s p o r t Theory Code DSN, (23) was b a s i c a l l y a multi-group transport calculation

i n c y l i n d r i c a l geometry, w i t h some Monte C a r l o a s s i s t a n c e i n t h e resolved resonance region. The i n t r o d u c t i o n of t h e THULE code was a

b i g s t e p i n t h e d i r e c t i o n of b a s i n g D 0 l a t t i c e c a l c u l a t i o n s on t r u l y

fundamental methods.
B.

C e l l c a l c u l a t i o n s Development

1.

U.S.

Methods An e x t e n s i v e comparison of c a l c u l a t i o n s and e x p e r i m e n t s was

p r e s e n t e d i n a 1964 review a r t i c l e by Honeck and C r a n d a l l . ( 4 )

6
An e x t e n s i v e c a l c u l a t i o n a l s t u d y of s i n g l e - r o d was p r e s e n t e d i n t h e review.

BNWL- 1119

uniform l a t t i c e s

I n t h i s s t u d y t h e computer codes

THERMOS ( I 8 ) and F R ( 2 4 ) were used t o g e n e r a t e few group c o n s t a n t s , OM and t h e e x p e r i m e n t a l b u c k l i n g was used t o d e s c r i b e l e a k a g e i n computing k eff The c a l c u l a t i o n s proved t o match t h e e x p e r i m e n t s

e x t r e m e l y c l o s e l y and a n immediate development program w a s undert a k e n by Honeck and J . E. S u i c h , of Savannah R i v e r L a b o r a t o r y , t o automate t h e p r o c e s s i n a s i n g l e c o m p u t a t i o n a l code. The r e s u l t was t h e H M E ( 2 5 ) code which h a s s i n c e become t h e A MR s t a n d a r d code f o r heavy w a t e r l a t t i c e c a l c u l a t i o n s i n many of t h e
U.S.

l a b o r a t o r i e s , and more r e c e n t l y h a s been a d a p t e d a l s o t o t h e Although t h e code r e t a i n s many a p p r o x i m a t i o n s

Chalk R i v e r computers.

i t i s b a s i c a l l y a f i r s t - p r i n c i p l e s method, working d i r e c t l y from t h e


r e a c t o r geometry and m a t e r i a l c r o s s s e c t i o n s w i t h o u t any e m p i r i c a l f i t t i n g factors. C a l c u l a t i o n s a r e made i n 84 e n e r g y g r o u p s , 30 i n

t h e t h e r m a l n e u t r o n energy r e g i o n (THERMOS)\18) and 54 i n t h e e p i ( t h e r m a l r e g i o n (MUFT) ,I 5 ) u s i n g i n t e g r a l t r a n s p o r t methods. Resonance c r o s s s e c t i o n s i n t h e e p i t h e r m a l r e g i o n a r e d e t e r m i n e d by built-in s i d e c a l c u l a t i o n s t h r o u g h t h e ZUT and TUZ codes. (26)

E x c e l l e n t agreement h a s been o b t a i n e d ( 2 7 ) between t h i s code and o v e r 100 e x p e r i m e n t s performed on s i n g l e r o d and t u b u l a r f u e l l a t t i c e s i n l a b o r a t o r i e s a l l over t h e world. T h i s agreement

s u p p l i e s a d e q u a t e p r o o f t h a t H M E i s c a p a b l e of p r o v i d i n g good A MR c a l c u l a t i o n s f o r uranium-D 0 l a t t i c e s w i t h s i m p l e f u e l geometry. 2 However, H M E i s a t p r e s e n t a one-dimensional A MR code, and can t r e a t

f u e l c l u s t e r s o n l y i n terms of s i m p l i f i e d c y l i n d e r i z e d models. These models h a v e t h e d i s a d v a n t a g e of n o t b e i n g a b l e s i m u l t a n e o u s l y

t o reproduce t h e c o r r e c t m a t e r i a l a r e a s , t h e c l u s t e r s i z e , t h e f u e l s u r f a c e s , and t h e s c a t t e r i n g p a t h s . Another m a j o r

l i m i t a t i o n of t h e HAMMER code i s i t s i n a d e q u a t e r e s o n a n c e t r e a t m e n t , s p e c i f i c a l l y t h e u s e o f t h e narrow r e s o n a n c e a p p r o x i m a t i o n f o r m o d e r a t o r and c o o l a n t , t h e n e g l e c t o f r e s o n a n c e o v e r l a p e f f e c t s , and t h e assumption o f a f l a t f l u x i n t h e r e s o n a n c e e n e r g y r e g i o n . Recent comparisons between HAMMER c a l c u l a t i o n s and f u e l c l u s t e r e x p e r i m e n t s show a p p r e c i a b l e d i f f e r e n c e s . I n s p i t e of i t s l i m i t a t i o n s , of D 0 2 Some work h a s

t h e H M E code r e p r e s e n t s t h e s t a t e - o f - t h e - t e c h n o l o g y A MR r e a c t o r physics c a l c u l a t i o n s i n t h e United S t a t e s .

been done u n d e r a USAEC-AECL c o o p e r a t i v e program toward d e v e l o p i n g a two-dimensional v e r s i o n of HAMMER, s p e c i f i c a l l y f o r f u e l c l u s t e r calculations. Another c a l c u l a t i o n a l scheme which r e p r e s e n t s t h e approach of a d a p t i n g codes developed f o r H 0 l a t t i c e s , i s t h a t developed by 2 Battelle-Northwest. T h i s scheme i s s i m i l a r t o HAMMER i n t h a t i t

u s e s t h e THERMOS code f o r t h e t h e r m a l i z a t i o n c a l c u l a t i o n , b u t d i f f e r s from H M E i n t h a t i t u s e s t h e code HRG (28) (Hanford A MR R e v i s e d G M for t h e slowing-down c a l c u l a t i o n . A ) The HRG-THERMOS

scheme, coupled w i t h a d i f f u s i o n t h e o r y r e a c t o r c a l c u l a t i o n , h a s been a p p l i e d a t B a t t e l l e - N o r t h w e s t w i t h a f a i r d e g r e e of s u c c e s s t o plutonium-fueled D 0 r e a c t o r s . 2 F o r e i g n Methods I n r e c e n t y e a r s i n B r i t a i n t h e THULE program h a s l e d t o t h e development of t h e W i n f r i t h Improved Multi-group Scheme, WIMS. (29)

The o p t i o n s i n c o r p o r a t e d i n t h e WIMS code a l l o w . t h e c a l c u l a t i o n

of s i m p l e l a t t i c e s w i t h any m o d e r a t o r , a s w e l l a s complex c l u s t e r systems with e i t h e r gas channels o r l i q u i d coolants.


It is a

h i g h l y f l e x i b l e code a l l o w i n g e i t h e r e l a b o r a t e c a l c u l a t i o n s i n many g r o u p s o r more r a p i d computations i n few groups f o r d e s i g n p u r p o s e s . The geometry o f a c l u s t e r c e l l can b e r e p r e s e n t e d by e i t h e r c o n c e n t r i c r i n g s o r an e x p l i c i t c o l l i s i o n p r o b a b i l i t y method which allows a d e t a i l e d r e p r e s e n t a t i o n of c l u s t e r geometries. The

t r e a t m e n t o f r e s o n a n c e s i n WIMS d i f f e r s from t h a t i n THULE ( 2 2 ) which r e q u i r e d e x p e n s i v e Monte C a r l o c a l c u l a t i o n s . The r e s o n a n c e t r e a t m e n t

i n WIMS i s b a s e d on e q u i v a l e n c e theorems which r e l a t e a l i b r a r y of r e s o n a n c e i n t e g r a l s f o r e a c h r e s o n a n c e a b s o r b e r i n e a c h g r o u p t o t h e p a r t i c u l a r h e t e r o g e n e o u s problem.


I t t a k e s a c c o u n t of

s o u r c e - d e p l e t i o n s w i t h i n g r o u p s caused by t h e r e s o n a n c e a b s o r p t i o n , and a c c o u n t of r e s o n a n c e i n t e r a c t i o n e f f e c t s .
A number o f methods

a r e a v a i l a b l e t o modify t h e i n f i n i t e l a t t i c e r e s u l t s t o i n c l u d e leakage i n a f i n i t e reactor. c a l c u l a t i o n s may b e performed. Both d i f f u s i o n and t r a n s p o r t t h e o r y The a c c u r a c y of t h e a p p r o x i m a t i o n s

used i n WIMS have been checked q u i t e e x h a u s t i v e l y by Monte C a r l o and o t h e r b a s i c methods. The Swedish, who h a v e s t r a d i t i o n a l l y r e l i e d h e a v i l y on r e c i p e s , h a v e i n r e c e n t y e a r s shown a n i n t e r e s t i n i n t e g r a l t r a n s p o r t t h e o r y calculations. The most s o p h i s t i c a t e d c a l c u l a t i o n a l code t h e y a r e

u s i n g c u r r e n t l y i s FLEF, (30) which i s a v e r s i o n of t h e B r i t i s h WIMS (29) code.


A t I s p r a , I t a l y , Euratom h a s developed t h e code PINOCCHIO, (31)

which i s of a p p r o x i m a t e l y t h e same o r d e r of s o p h i s t i c a t i o n as

HAMMER. (25)

They a r e working on a two-dimensional r e p r e s e n t a t i o n

of c l u s t e r s f o r t h e THERMOS p o r t i o n of PINOCCHIO.
I t i s o b v i o u s from t h e above t h a t i n r e c e n t y e a r s t h e r e h a s

b e e n a world-wide

t r e n d away from r e c i p e methods and toward more

s o p h i s t i c a t e d c a l c u l a t i o n a l methods.
C.

B a s i c Data and Methods Used i n C a l c u l a t i o n s

A s t h e c a l c u l a t i o n a l methods become more r e f i n e d , and as t h e y a r e


b a s e d more and more on b a s i c p r i n c i p l e s , t h e need f o r a c c u r a t e c r o s s s e c t i o n i n f o r m a t i o n , s l o w i n g down t h e o r y , and s c a t t e r i n g k e r n e l s becomes more a c u t e . The f o l l o w i n g reviews p r e s e n t t h e s t a t e - o f - t h e -

technology i n t h e s e a r e a s of b a s i c d a t a and methods.

1.

Cross S e c t i o n s

( C o n t r i b u t e d by B. R. Leonard, Jr. and R.C.

Liikala)

Many of t h e c r o s s s e c t i o n s used today were p r e p a r e d i n t h e l a t e 1 9 5 0 ' s and have n e v e r b e e n updated. I n some c a s e s , t h e s e

d a t a a r e s t i l l t h e b e s t a v a i l a b l e , b u t i n most c a s e s b e t t e r d a t a exist. F u r t h e r m o r e , new measurements a r e b e i n g made a t an B e f o r e t h e d a t a can b e u t i l i z e d i n t h e r e a c t o r

increasing r a t e .

c a l c u l a t i o n , t h e e x p e r i m e n t a l d a t a must b e e v a l u a t e d i n t o p o i n t cross-section s e t s , and t h e p o i n t c r o s s - s e c t i o n s e t s p r o c e s s e d T h i s c a u s e s an a p p r e c i a b l e d e l a y between

i n t o multi-group s e t s .

measurement of t h e d a t a and u t i l i z a t i o n . The USAEC h a s i n i t i a t e d an i n t e n s e n a t i o n a l e f f o r t t o reduce t h e delays. New e v a l u a t e d p o i n t c r o s s - s e c t i o n s e t s h a v e

b e e n and a r e b e i n g p r e p a r e d , and p l a c e d i n a uniform f o r m a t known a s t h e ENDFIB system. (55) The work i s b e i n g done u n d e r t h e

10

BNWL- 1119

d i r e c t i o n of t h e Cross S e c t i o n E v a l u a t i o n Working Group, whose E members r e p r e s e n t some e i g h t e e n A C c o n t r a c t o r s , t h e Cross S e c t i o n E v a l u a t i o n C e n t e r a t BNL, and some o t h e r i n t e r e s t e d laboratories.
A number o f computer codes have b e e n d e v e l o p e d t o

p r o c e s s t h e ENDFIB d a t a i n t o multi-group codes are now o p e r a t i o n a l and multi-group

sets.

Many o f t h e s e

s e t s a r e being generated.

I n c l u d e d i n t h e ENDFIB d a t a a r e t h e r m a l s c a t t e r i n g laws f o r most o f t h e m a t e r i a l s used i n heavy w a t e r r e a c t o r s . This collection

of d a t a w i l l make i t p o s s i b l e t o e x p l i c i t l y compare c a l c u l a t i o n a l methods u s e d a t v a r i o u s l a b o r a t o r i e s by u s i n g t h i s s e t of b a s i c n u c l e a r d a t a w i t h t h e v a r i o u s methods.


A b r i e f review of t h e t h e r m a l and r e s o n a n c e c r o s s s e c t i o n s

f o r some of t h e f i s s i l e and f e r t i l e n u c l i d e s i m p o r t a n t t o D 0 2 reactors a r e given here.


a.

Thermal.

The p r e c i s i o n of t h e knowledge o f t h e t h e r m a l

c r o s s s e c t i o n v a l u e s of p l u t o n i u m h i s t o r i c a l l y h a s b e e n i n f e r i o r t o t h a t o f uranium. The e v a l u a t i o n s of 2200 m/sec

v a l u e s f o r 2 3 2 ~ hand 2 3 8 ~ r e g e n e r a l l y w i t h i n t h e band of a u n c e r t a i n t y +2%. Only two p r e c i s e m o n o e n e r g e t i c measurements e x i s t of t h e 2200 m l s e c a b s o r p t i o n c r o s s s e c t i o n of 2 4 0 ~ u and t h e s e d i f f e r by 5.4%. v a l u e s of P r e c i s i o n s i n t h e fundamental

and a f o r p l u t o n i u m 239 and 241 a r e f a c t o r s of A d d i t i o n a l and

%5 worse t h a n f o r uranium 233 and 235.

related uncertainties a r e present i n calculating reaction r a t e s i n r e a c t o r s p e c t r a f o r systems containing plutonium because o f a s i g n i f i c a n t l y non-l/v b e h a v i o r of t h e t h e r m a l c r o s s s e c t i o n of t h e p r i n c i p a l f i s s i l e i s o t o p e s , 2 3 9 ~ uand 241F'~,

Various a d j u s t m e n t s i n t h e 2200 m/sec v a l u e s of t h e m a j o r f i s s i l e - n u c l i d e c o n s t a n t s h a v e b e e n made s i n c e 1961.


A t t h e p r e s e n t t i m e , t h e IAEA i s s p o n s o r i n g a n o t h e r

a d j u s t m e n t which w i l l i n c o r p o r a t e t h e r e s u l t s o f a dozen o r s o measurements completed s i n c e t h e l a s t e v a l u a t i o n i n 1965. The a d j u s t m e n t i s e x p e c t e d t o b e completed i n t h e While t h e f o r t h c o m i n g a d j u s t e d c o n s t a n t s

s p r i n g of 1969.

w i l l p r o b a b l y b e t h e b e s t e s t i m a t e of t h e v a l u e s a t t h a t time t h e p r e c i s i o n s which w i l l b e a s s i g n e d s h o u l d b e c a r e f u l l y considered. One o f t h e most p r o m i s i n g approaches t o improving t h e knowledge of t h e c r o s s s e c t i o n v a l u e s of t h e f i s s i l e n u c l i d e s


i s a s t u d y of spectrum-averaged

o r e f f e c t i v e cross-section In the

measurements w i t h modern c a l c u l a t i o n a l methods.

p a s t such e x p e r i m e n t s h a v e b e e n a l m o s t u n i v e r s a l l y i n t e r p r e t e d i n terms o f t h e Maxwellian t h e r m a l spectrum. u n c e r t a i n t i e s due t o d e v i a t i o n s from a Maxwellian s h a p e a r e n o t a s s e s s e d i n such an i n t e r p r e t a t i o n . In addition, The

t h e r e e x i s t s t h e r e l a t e d u n c e r t a i n t y of compounding t h e e r r o r by u s i n g 2200 m/sec v a l u e s d e r i v e d on t h e assumption of a Maxwellian s h a p e and t h e n c a l c u l a t i n g r e a c t i o n r a t e s u s i n g c a l c u l a t i o n a l codes which do n o t assume a Maxwellian spectrum. b. Resonance. 232Th, 238iJ, The u n c e r t a i n t y i n t h e r e s o n a n c e c r o s s s e c t i o n s f o r and 2 4 0 ~ u s perhaps no g r e a t e r t h a n 5%. i The

c a l c u l a t e d values o f t h e resonance i n t e g r a l s f o r i n f i n i t e d i l u t i o n b a s e d upon d i f f e r e n t i a l c r o s s s e c t i o n s when compared

12

B W - 1119 N L

t o d i r e c t l y measured v a l u e s g e n e r a l l y a g r e e t o w i t h i n

'4%f0r

2 32 T h a n d 238Uand a b o u t f 5 % f ~ r ~ ~ O PHowever, u .

based upon c a l c u l a t e d resonance i n t e g r a l s f o r 2 3 8 ~ d i f f e r e n t i a l d a t a a r e c o n s i s t e n t l y lower t h a n d i r e c t l y measured v a l u e s ( i . e . , c a l c u l a t e d %270 b , measured %282).

The complexity of t h e r e s o n a n c e s t r u c t u r e f o r t h e s e n u c l i d e s adds t o t h e u n c e r t a i n t y i n c a l c u l a t i n g t h e r e a c t i o n r a t e s i n thermal r e a c t o r s , with t h e 2 4 0 r e a c t i o n r a t e being t h e ~ ~ most d i f f i c u l t t o c a l c u l a t e . A d d i t i o n a l e f f o r t s a r e needed t o p u t t h i s t e c h n o l o g y on f i r m ground. The s y s t e m a t i c d i f f e r e n c e between measured

and c a l c u l a t e d v a l u e s of t h e 2 3 8 ~ e s o n a n c e i n t e g r a l n e e d s r t o be resolved. More m o n o e n e r g e t i c measurements of t h e

2 4 0 ~ uc r o s s s e c t i o n s a r e d e s i r a b l e . 2. Slowing Down Treatment i n Heavy Water R e a c t o r s


J. L.

(Contributed by

Carter, Jr.)

Many o f t h e e p i t h e m a l c a l c u l a t i o n s f o r D 0 s y s t e m s have 2 b e e n done w i t h t h e MUFT ( I 5 ) code, o r o t h e r s b a s e d on i t s t e c h n i q u e . Briefly, t h i s technique solves the B

or P

v e r s i o n of t h e

homogenized Boltzmann t r a n s p o r t e q u a t i o n , u s i n g t h e a u x i l i a r y c o n c e p t of s l o w i n g down d e n s i t y . Slowing down by hydrogen i s

t r e a t e d e x a c t l y and s l o w i n g down by o t h e r atoms may b e t r e a t e d by t h e Greuling-Goert z e l (56) method. Corrections f o r resonance

a b s o r p t i o n a r e made u s i n g a form f o r r e s o n a n c e i n t e g r a l s d e r i v e d f o r unbroadened r e s o n a n c e s i n a homogenized s y s t e m , b u t w i t h t h e p o s s i b i l i t y of m o d i f y i n g some of t h e p a r a m e t e r s t o a l l o w

f o r h e t e r o g e n e i t y and Doppler b r o a d e n i n g t o a low o r d e r of approximation. The t e c h n i q u e was d e r i v e d o r i g i n a l l y f o r u s e

i n H 0 s y s t e m s , f o r which t h e a p p r o x i m a t i o n s a r e more v a l i d 2 than f o r D 0 systems. 2 I n p r a c t i c e , t h e t e c h n i q u e h a s proved

q u i t e a c c e p t a b l e f o r b o t h s y s t e m s , ( 4 ) e s p e c i a l l y when c a l i b r a t e d t o s t u d y v a r i a t i o n s of a s p e c i f i c c o n c e p t . Although t h e G r e u l i n g - ~ o e r t z e l method i s a g r e a t improvement o v e r Fermi a g e t h e o r y f o r d e u t e r i u m , i t g i v e s o n l y a rough d e s c r i p t i o n o f t h e s c a t t e r i n g p r o p e r t i e s of deuterium. Since

t h e r e s o n a n c e t r e a t m e n t i n MUFT i s a l s o q u i t e a p p r o x i m a t e , t h e o v e r a l l s u c c e s s of t h e a n a l y s i s of D 0 s y s t e m s , u s i n g MUFT 2 f o r t h e e p i t h e r m a l r e g i o n , may b e a t t r i b u t e d t o two f a c t o r s : t h e s u b o r d i n a t e r o l e t h e epithermal r e g i o n plays i n such systems and a f o r t u i t o u s b a l a n c i n g of a p p r o x i m a t i o n e r r o r s . Though

t h i s s u c c e s s i s e n c o u r a g i n g f o r t h e adequacy of f u r t h e r c a l c u l a t i o n s on s i m i l a r s y s t e m s , d o u b t s a r i s e as t o t h e a c c u r a c y of c a l c u l a t i o n s on d i f f e r e n t , and more complex s y s t e m s , f o r example t h o s e u s i n g plutonium a s f u e l , l i g h t w a t e r a s c o o l a n t , and heavy w a t e r a s t h e m o d e r a t o r . Comparison of r e s u l t s o b t a i n e d

u s i n g t h e MUFT t e c h n i q u e w i t h t h o s e o b t a i n e d u s i n g d i f f i c u l t and improved t e c h n i q u e s seem i n d i c a t e d . S e v e r a l e p i t h e r m a l s p e c t r u m codes a l r e a d y e x i s t which u s e t e c h n i q u e s d i f f e r e n t from, and improved upon, t h e MUFT t e c h n i q u e . The e p i t h e r m a l p o r t i o n of t h e HAMMER ( 2 5 ) s y s t e m u s e s t h e MUFT s l o w i n g down t e c h n i q u e i n a h e t e r o g e n e o u s c a l c u l a t i o n b a s e d on i n t e g r a l t r a n s p o r t t h e o r y and h a s a n improved r e s o n a n c e

14

B W - 1 19 N L 1

t r e a t m e n t which i n c l u d e s h e t e r o g e n e i t y and Doppler b r o a d e n i n g effects. The GAM-I, ( 5 7 ) GAM-I1 and HRG (28) ( a n improved v e r s i o n

o f t h e GAM-I)

codes, use a f u l l s c a t t e r i n g t r a n s f e r m a t r i x ,

r a t h e r than t h e Greuling-Goertzel approximation, i n s o l v i n g the B

or P

v e r s i o n of t h e homogenized Boltzmann t r a n s p o r t

equation.

Treatment of r e s o n a n c e s i n t h e s e codes i s by t h e

Adler-Nordheim (58) t e c h n i q u e and i n c l u d e s h e t e r o g e n e i t y and Doppler b r o a d e n i n g .


A comparison of a n a l y s e s o f s i m p l e D 0 2

s y s t e m s u s i n g t h e d i f f e r e n t t e c h n i q u e s of HRG and H M E would A MR e v a l u a t e two d i f f e r e n t a p p r o a c h e s t o t r e a t i n g s l o w i n g down and r e s o n a n c e a b s o r p t i o n . To b e s i g n i f i c a n t , t h e comparison

s h o u l d b e made u s i n g n u c l e a r d a t a from t h e same c o m p i l a t i o n , e.g., t h e BNW M a s t e r L i b r a r y o r t h e

ENDFIB (55)

d a t a system.

3.

The E x p e r i m e n t a l S c a t t e r i n g Law f o r Heavy Water ( c o n t r i b u t e d by 0 . K. H a r l i n g ) a. Introduction

I n o r d e r t o c a r r y o u t t h e r m a l i z a t i o n c a l c u l a t i o n s , energy t r a n s f e r c r o s s s e c t i o n s must b e known f o r a comprehensive g r i d of e n e r g y and momentum changes. Measurements a r e made

o f t h e d o u b l e d i f f e r e n t i a l c r o s s s e c t i o n a ( E +E ,0) which i s 0 1 r e l a t e d t o t h e s c a t t e r i n g law, ( 5 9 ) S(a,B) by t h e f o l l o w i n g relations,

m[Eo o
= ( A P / ~ M ~=T ) ~

El

~ ( E ~ E , ) " os0] c~ (1)

MkT

15 where E and E

B W - 1119 N L

a r e t h e f i n a l and i n i t i a l n e u t r o n e n e r g i e s ,

8 i s t h e s c a t t e r i n g a n g l e , m i s t h e n e u t r o n mass, M i s t h e mass of t h e p r i n c i p a l s c a t t e r i n g atom, k i s Boltzmann's c o n s t a n t and


T i s t h e a b s o l u t e temperature.

Experimental determinations of

a(Eo+E1,8),

g e n e r a l l y p r o v i d e r e s u l t s f o r a l i m i t e d r a n g e of S i n c e t h e r e i s f r e q u e n t l y no

momentum and energy changes.

r a p i d l y varying s t r u c t u r e i n t h e cross s e c t i o n s f o r moderators, s i m p l e i n t e r p o l a t i o n can o f t e n b e used t o p r o v i d e a more comprehensive g r i d i n A and AE. P However, i t i s d e s i r a b l e t o

d e v e l o p a s c a t t e r i n g law o r s c a t t e r i n g k e r n e l which can p r o v i d e s l o w i n g down c r o s s s e c t i o n s f o r any v a l u e of energy and momentum t r a n s f e r f o r t h e e n t i r e r a n g e of t h e s e v a r i a b l e s which i s of i n t e r e s t i n t h e r m a l i z a t i o n problems. T h i s can o f t e n b e done

w i t h t h e a i d of t h e o r e t i c a l models which have b e e n a d j u s t e d t o f i t e x p e r i m e n t a l r e s u l t s o v e r t h e l i m i t e d r a n g e s i n which t h e . d a t a are available. The s t a t u s of t h e D 0 s c a t t e r i n g law w i l l

b e d i s c u s s e d h e r e w i t h r e f e r e n c e t o t h e t y p e and c o v e r a g e of e x i s t i n g e x p e r i m e n t a l r e s u l t s , t h e c o n s i s t e n c y and a c c u r a c y of r e s u l t s , p o s s i b l e s o u r c e s of e r r o r s i n measurements and comp a r i s o n of e x p e r i m e n t a l s c a t t e r i n g law w i t h r e s u l t s from model calculations.


b.

E x p e r i m e n t a l Cross S e c t i o n s f o r D 0 2 Double d i f f e r e n t i a l c r o s s s e c t i o n s measurements u s i n g t h e s l o w n e u t r o n d o w n s c a t t e r i n g t e c h n i q u e , p r o v i d e t h e most e x t e n s i v e s e t s o f measured s l o w i n g down c r o s s s e c t i o n s . e x p e r i m e n t a l s t u d i e s of t h i s t y p e have b e e n made on D 0 . Several

16

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Haywood (60) used a phased m u l t i p l e r o t o r chopper t o measure t h e s c a t t e r i n g law f o r 2 9 5 ' ~ and 423K heavy w a t e r w i t h b e t a v a l u e s t o -3 and ct v a l u e s t o ~ 6 . Using t h e same s p e c t r o m e t e r Page (61) h a s measured t h e s c a t t e r i n g law f o r a 540K heavy w a t e r sample and h a s p u b l i s h e d a c o m p i l a t i o n which i n c l u d e s S(ct,B) v a l u e s f o r
f3 t o -1.85

and ct v a l u e s t o ~ 5 . H a r l i n g ( 6 2 ) h a s r e p o r t e d

measurements of t h e s c a t t e r i n g law f o r 2 9 9 ' ~D 0 , u s i n g a 2 r o t a t i n g c r y s t a l s p e c t r o m e t e r , w i t h f3 v a l u e s t o -7.5 1 5 and a's to

High energy t r a n s f e r measurements a t 2 9 4 ' ~ u s i n g a n ~

e l e c t r o n l i n e a r a c c e l e r a t o r h a v e b e e n r e p o r t e d by Whittemore, (63) w i t h f3 v a l u e s t o -25 and


ct

values t o ~ 4 0 .

I n e x p e r i m e n t a l r e s u l t s o f t h i s t y p e , i n v o l v i n g complex m e a s u r i n g t e c h n i q u e , t h e q u e s t i o n of a c c u r a c y i s a n i m p o r t a n t one. T h i s i s e s p e c i a l l y t r u e i n t h e c a s e o f m o d e r a t o r s c a t t e r i n g laws s i n c e t h e d a t a may b e used t o p r e d i c t n e u t r o n i c s b e h a v i o r of e x p e n s i v e r e a c t o r systems. One good measure o f t h e q u a l i t y of

e x p e r i m e n t a l r e s u l t s i s t h e c o n s i s t e n c y of r e s u l t s from a s i n g l e laboratory. Where measurements of t h e same q u a n t i t y h a v e b e e n

o b t a i n e d by d i f f e r e n t i n v e s t i g a t o r s and l a b o r a t o r i e s a b e t t e r t e s t of a c c u r a c y i s t o compare t h e s e i n d e p e n d e n t r e s u l t s .
A measure of t h e e x i s t i n g a c c u r a c y i n t h e measured room

t e m p e r a t u r e s c a t t e r i n g law f o r D 0 , c a n b e o b t a i n e d by comparing 2 t h e i n d e p e n d e n t r e s u l t s o f Haywood, (60) Whittemore (63) and Harling

.(62)(93)

I t i s c l e a r t h a t s u b s t a n t i a l d i f f e r e n c e s e x i s t between t h e

v a r i o u s sets of d a t a and i n some c a s e s t h e r e i s a l s o c o n s i d e r a b l e d i s p e r s i o n w i t h i n a s i n g l e s e t of d a t a . Near t h e p e a k s

of t h e s ( a , B ) c u r v e s t h e t o t a l s p r e a d i n S v a l u e s i s a p p r o x i m a t e l y 58, 38, 1 9 and 33% r e s p e c t i v e l y f o r t h e c u r v e s a t

1, 3, 5 , and 7.

The mean t o t a l s p r e a d i s %37%. Somewhat

l a r g e r s p r e a d s o c c u r a t t h e low and h i g h a ends of t h e d a t a sets. With a view toward u l t i m a t e u s e i n r e a c t o r t h e r m a l i z a t i o n

c a l c u l a t i o n s a b e t t e r gauge of t h e c o n s i s t e n c y between s e p a r a t e s e t s of e x p e r i m e n t a l d a t a might b e t o f i t smooth c u r v e s t o e a c h set of d a t a and t h e n o b t a i n a mean by a v e r a g i n g t h e s e p a r a t e curves. T h i s t e n d s t o smooth o u t any f i n e s t r u c t u r e i n

a b u t should be s a t i s f a c t o r y f o r t h e thermalization k e r n e l i n t h e c a s e of D 0 . 2 Using t h i s p r o c e d u r e t o o b t a i n s e v e r a l a v e r a g e

d a t a p o i n t s n e a r t h e peaks of t h e S c u r v e s w e f i n d mean v a l u e s which h a v e a n rms d e v i a t i o n o f about 23, 4, 7.5 and 5 % , r e s p e c t i v e l y f o r t h e c u r v e s w i t h B = 1, 3 , 5, and 7 . This

magnitude of s p r e a d i n S f o r measurements t a k e n a t d i f f e r e n t l a b o r a t o r i e s i s r e p r e s e n t a t i v e of t h e p r e s e n t s t a t e of t h e a r t i n measurements of t h i s t y p e . Approximately t h e same d e g r e e

o f i n c o n s i s t e n c y i s found i n room t e m p e r a t u r e l i g h t water measurements a t t h i s t i m e . (62,64,65)

E x t e n s i v e r e s u l t s f o r S(a,B) a t e l e v a t e d t e m p e r a t u r e s a r e a v a i l a b l e o n l y from one l a b o r a t o r y , t h e Atomic Energy E s t a b l i s h ment, H a r w e l l , England.(60y61) The s c a t t e r of t h e i n d i v i d u a l

d a t a p o i n t s i s w i t h i n a b o u t 25% f o r t h e v a r i o u s measurements. c. Source o f E r r o r i n E x p e r i m e n t a l R e s u l t s The e x p e r i m e n t a l r e s u l t s a r e s u b j e c t t o a number o f s o u r c e s of e r r o r . The most i m p o r t a n t o f t h e s e a r e b e l i e v e d t o b e :

a) b) c) d)

S t a t i s t i c a l counting e r r o r s Resolution e f f e c t s Multiple scattering Various s y s t e m a t i c e r r o r s

The c o u n t i n g s t a t i s t i c s a r e e a s y enough t o d e t e r m i n e d u r i n g t h e r e d u c t i o n of t h e raw d a t a t o c r o s s s e c t i o n s . This e r r o r i s

u s u a l l y s m a l l compared t o t h e s c a t t e r of t h e d a t a from t h e v a r i o u s experiments. Also, t h e randomness of d i r e c t i o n of t h i s

e r r o r i n s u r e s t h a t t h e r e is no systematic b i a s i n t h e r e s u l t s and a l l one n e e d s t o do t o make t h i s e r r o r s m a l l i s t o o b t a i n s u f f i c i e n t measurements o r c o u n t s . R e s o l u t i o n e f f e c t s a r e of two t y p e s , t h o s e due t o r e s o l u t i o n i n a n g l e and t h o s e due t o e n e r g y r e s o l u t i o n . The f o r m e r a f f e c t s

t h e s t r u c t u r e i n momentum t r a n s f e r and i s n o t g e n e r a l l y i m p o r t a n t f o r moderator m a t e r i a l s w i t h t h e commonly u t i l i z e d counter s o l i d angles. important factor. The e n e r g y r e s o l u t i o n i s , however, an
(TOF)

I n general, f o r a time-of-flight

s p e c t r o m e t e r t h e r e s o l u t i o n on e n e r g y t r a n s f e r i s s t r o n g l y dependent upon t h e e n e r g y t r a n s f e r . For a g i v e n i n i t i a l e n e r g y

t h e l a r g e s t e n e r g y t r a n s f e r s a r e measured w i t h t h e b e s t r e s o l u t i o n w h i l e s m a l l e n e r g y changes have t h e w o r s t resolution. The s i t u a t i o n i s p a r t i c u l a r l y bad n e a r t h e q u a s i In principle

e l a s t i c peak i n t h e s c a t t e r e d n e u t r o n spectrum.

i t i s p o s s i b l e t o remove t h e q u a s i e l a s t i c s c a t t e r i n g peak from

t h e d o w n s c a t t e r e d spectrum. w i t h t h e r e q u i r e d accuracy.

However, t h i s i s d i f f i c u l t t o do I n practice i t is highly d e s i r a b l e

t o design t h e experiments t o provide d a t a f o r over-lapping energy t r a n s f e r s . When t h i s i s done i t i s p o s s i b l e t o choose

t h e d a t a f o r a g i v e n I3 v a l u e which i s l e a s t l i k e l y t o be s u b j e c t t o r e s o l u t i o n b r o a d e n i n g o r o t h e r s o u r c e s of e r r o r , e . g . , m u l t i p l e s c a t t e r i n g which w i l l b e d i s c u s s e d below. The

p r e s e n t l y a v a i l a b l e d a t a on D 0 h a s p r o b a b l y been t a k e n w i t h 2 a d e q u a t e e n e r g y r e s o l u t i o n t o produce an a d e q u a t e s c a t t e r i n g k e r n e l , w i t h t h e p o s s i b l e e x c e p t i o n of v e r y low e n e r g y t r a n s f e r data. The r e s u l t s c i t e d above w e r e n o t o b t a i n e d w i t h good from %O t o % . 5 . Cold n e u t r o n

r e s o l u t i o n i n t h e region of

u p s c a t t e r i n g e x p e r i m e n t s w i t h b e r y l l i u m f i l t e r e d n e u t r o n s have p o t e n t i a l l y v e r y good r e s o l u t i o n i n t h i s low e n e r g y t r a n s f e r r e g i o n and c o u l d b e used t o supplement t h e d o w n s c a t t e r i n g results. Measurements of t h i s t y p e h a v e been made on D 0 by 2

L a r s s o n and Dahlborg. ( 6 6 ) The m u l t i p l e s c a t t e r i n g o f n e u t r o n s w i t h t h e " t y p i c a l " samples produce e r r o r s i n t h e s c a t t e r i n g d i s t r i b u t i o n s which a r e e x p e c t e d t o v a r y from f r a c t i o n a l l y l a r g e t o f r a c t i o n a l l y n e g l i g i b l e , depending upon t h e a and I3 v a l u e a t which t h e n e u t r o n
i s o b s e r v e d and upon t h e s c a t t e r i n g p r o p e r t i e s o r t r u e s c a t t e r -

i n g law f o r t h e sample.

I t h a s b e e n found by S l a g g i e ( 6 7 ) t h a t

even with r e l a t i v e l y high transmission t h e m u l t i p l y s c a t t e r e d f l u x i n H 0 e x p e r i m e n t s can a c c o u n t f o r a l a r g e f r a c t i o n o f t h e 2 measured c r o s s s e c t i o n s , e . g . ,


%30% f o r some v a l u e s of a

and B

The l a r g e s t c o r r e c t i o n s a p p l y f o r s m a l l momentum t r a n s f e r s and l a r g e v a l u e s of e n e r g y t r a n s f e r . The S l a g g i e c o m p u t a t i o n a l

scheme f o r w a t e r i s b a s e d on an i n c o h e r e n t s c a t t e r e r and t h e r e f o r e i s n o t n e c e s s a r i l y a p p l i c a b l e t o D 2 0 which h a s a p r i m a r i l y coherent s c a t t e r i n g cross s e c t i o n . However, r e c e n t work by

Haywood and Page (68) and by ~ a r l i n ~ ' ~ i' n d i c a t e s t h a t s c a t t e r ) i n g from D 0 c a n b e w e l l d e s c r i b e d w i t h o u t e x p l i c i t a t t e n t i o n 2 t o coherence e f f e c t s . Therefore, the multiple s c a t t e r i n g

c o r r e c t i o n s c a l c u l a t e d by S l a g g i e f o r l i g h t w a t e r a r e p r o b a b l y r e a s o n a b l e e s t i m a t e s of t h e same e f f e c t i n D 0. 2 I n view of t h e

magnitude of t h e m u l t i p l e s c a t t e r i n g c o r r e c t i o n s and t h e s e n s i t i v i t y of t h e e f f e c t t o e x p e r i m e n t a l p a r a m e t e r s l i k e sample t h i c k n e s s , i n i t i a l and f i n a l e n e r g y and s c a t t e r i n g a n g l e , a r e a l l y good comparison of p r e s e n t l y a v a i l a b l e d a t a i s n o t possible.


I t seems d e s i r a b l e , t h e r e f o r e , t o make t h e b e s t

possible multiple scattering corrections t o the available data b e f o r e t h e s e a r e used t o d e r i v e a s t a t e - o f - t h e - a r t k e r n e l f o r D20. V a r i o u s o t h e r s o u r c e s of e r r o r may b e p r e s e n t i n d o u b l e d i f f e r e n t i a l cross section results. These i n c l u d e e r r o r s due scattering

t o background s u b t r a c t i o n , i n n o r m a l i z a t i o n t o o b t a i n a b s o l u t e c r o s s s e c t i o n s , t h e d e t e c t o r response function, contamination o f t h e i n c i d e n t beam, a i r s c a t t e r i n g i n t h e d e t e c t o r f l i g h t p a t h s , u n c e r t a i n t i e s i n t h e sample c o m p o s i t i o n o r s i z e and v a r i o u s i n s t r u m e n t a l problems which o c c u r i n a l m o s t e v e r y experiment. I n g e n e r a l , i t s h o u l d b e p o s s i b l e t o make t h e

i n f l u e n c e of t h e s e f a c t o r s s m a l l compared t o t h e e f f e c t s of multiple scattering or resolution effects. However, t h e r e i s

always a p o s s i b i l i t y t h a t a s y s t e m a t i c s o u r c e of e r r o r may

o c c u r which i s e i t h e r i n a d e q u a t e l y c o r r e c t e d o r which i s n o t recognized a t a l l . d. E x p e r i m e n t a l R e s u l t s Compared w i t h Model C a l c u l a t i o n s Various models have been developed t o c a l c u l a t e t h e s c a t t e r i n g from D 0 . 2 One of t h e b e s t t e s t s o f t h e a c c u r a c y of s u c h

a model i s t o u s e i t t o c a l c u l a t e c r o s s s e c t i o n s which can b e compared t o e x p e r i m e n t a l v a l u e s . I n doing t h i s i t should b e

remembered t h a t t h e e x p e r i m e n t a l r e s u l t s a r e i n some c a s e s s u b j e c t t o s u b s t a n t i a l s o u r c e s of e r r o r . Two models which have

been m o d e r a t e l y s u c c e s s f u l i n p r e d i c t i n g t h e s c a t t e r i n g p r o p e r t i e s of D 0 a r e : 1 ) t h e McMurry-Russell ( 7 0 ) model f o r 2 w a t e r which i s a r e f i n e m e n t of t h e

elki in'^')

model and which

h a s b e e n a d a p t e d t o heavy w a t e r , ( 7 2 ) and 2 ) a model b a s e d on t h e t h e o r e t i c a l approach of E g e l s t a f f and S c h o f i e l d (73) which uses an incoherent theory w i t h a Gaussian approximation t o t h e self-correlation. I n t h e Egelstaff-Schofield theory t h e

s c a t t e r i n g law i s c a l c u l a t e d from a multiphonon e x p a n s i o n u s i n g t h e computer program LEAP (74) and a s p e c t r a l d e n s i t y f u n c t i o n which can b e d e r i v e d from e x p e r i m e n t s o r from t h e o r e t i c a l considerations. The r a t h e r l a r g e d i f f e r e n c e between t h e t h e o r e t i c a l s c a t t e r i n g law v a l u e s and t h e e x p e r i m e n t a l r e s u l t s a t s m a l l a v a l u e s

i s d i s t u r b i n g and i n d i c a t e s a need f o r a n u n d e r s t a n d i n g r e g a r d i n g i t s source.


I t would b e d e s i r a b l e t o make c o r r e c t i o n s t o t h e The i n -

d a t a f o r m u l t i p l e s c a t t e r i n g and r e s o l u t i o n e f f e c t s . f l u e n c e of coherence should a l s o b e considered.

B u t l e r (75

22

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4.

S c a t t e r i n g K e r n e l s f o r Heavy Water ( c o n t r i b u t e d by Alan G * Gibbs) a. Introduction When s l o w n e u t r o n s i n t e r a c t w i t h a s y s t e m of atoms, t h e i n t e r a c t i o n s r e q u i r e s u f f i c i e n t time f o r t h e neutrons t o s e n s e n o t o n l y t h e p r e s e n c e , b u t a l s o t h e v e l o c i t i e s and a c c e l e r a t i o n s of t h e i n d i v i d u a l atoms. Thus b o t h s c a t t e r -

i n g and a b s o r p t i o n c r o s s s e c t i o n s f o r slow n e u t r o n s depend i n t i m a t e l y on t h e d e t a i l e d dynamics of t h e a t o m i c m o t i o n s . The dynamics of even an i s o l a t e d H 0 o r D 0 m o l e c u l e 2 2

i s complex, s i n c e t h e m o l e c u l e a s a whole can e x p e r i e n c e


b o t h t r a n s l a t i o n and r o t a t i o n , w h i l e t h e i n d i v i d u a l atoms can p a r t i c i p a t e c o l l e c t i v e l y i n t h r e e i n d e p e n d e n t v i b r a t i o n a l modes. A l l of t h e s e d e g r e e s of freedom may b e i n v o l v e d t o

some e x t e n t when a n e u t r o n i s s c a t t e r e d by t h e m o l e c u l e , The s i t u a t i o n i s f u r t h e r c o m p l i c a t e d i n problems o f p r a c t i c a l i n t e r e s t , s i n c e t h e molecules a r e n o t i s o l a t e d but occur i n water o r i c e . Here t h e i n t e r a c t i o n s between

n e i g h b o r i n g m o l e c u l e s l e a d t o a h i g h l y complex m u t u a l h i n d r a n c e of t h e i r t r a n s l a t i o n a l and r o t a t i o n a l motion. p r e c i s e d e s c r i p t i o n of t h i s p r o c e s s i s , of c o u r s e , n o t a v a i l a b l e , and c a l c u l a t i o n s of s c a t t e r i n g c r o s s s e c t i o n s must b e b a s e d on g r e a t l y s i m p l i f i e d models which ( h o p e f u l l y ) r e t a i n t h e e s s e n t i a l f e a t u r e s of t h e a c t u a l s y s t e m s , Some i m p o r t a n t s i m p l i f i c a t i o n s o c c u r i n d e s c r i b i n g s c a t t e r i n g by H 0 which do n o t o c c u r i n D20. 2 When n e u t r o n
A

waves a r e s c a t t e r e d by any a t o m i c n u c l e u s t h e p h a s e s h i f t

23 and Koppel and Young


(76)

B W - 1119 N L

h a v e shown t h a t t h e r e i s some c a n c e l -

l a t i o n i n t h e coherent s c a t t e r i n g but t h a t t h e s e e f f e c t s a r e
s t i l l l i k e l y t o be important i n t h e p a r t i a l cross s e c t i o n s a t

s m a l l a and B . e. Summary E x t e n s i v e room t e m p e r a t u r e d a t a e x i s t f o r t h e s c a t t e r i n g k e r n e l of D20. B e f o r e a v e r a g i n g t h e r e s u l t s from t h e s e p a r a t e scattering Especially

l a b o r a t o r i e s t o produce a s t a t e - o f - t h e - t e c h n o l o g y k e r n e l , c o r r e c t i o n s must b e a p p l i e d t o t h e d a t a .

i m p o r t a n t i s t h e q u e s t i o n of m u l t i p l e s c a t t e r i n g f o r which l a r g e c o r r e c t i o n s may b e n e c e s s a r y . Experimental r e s u l t s f o r D 0 s c a t t e r i n g a t e l e v a t e d 2 t e m p e r a t u r e s , a r e a v a i l a b l e o n l y f o r a l i m i t e d r a n g e of e n e r g y and momentum t r a n s f e r s . P r e s e n t l y a v a i l a b l e measurements do

n o t i n c l u d e t h e energy t r a n s f e r range of t h e i n t r a m o l e c u l a r v i b r a t i o n s which become more i m p o r t a n t i n t h e t h e r m a l i z a t i o n problem, t h e h i g h e r t h e m o d e r a t o r t e m p e r a t u r e . Also, t h e

e l e v a t e d t e m p e r a t u r e r e s u l t s a r e from o n l y one l a b o r a t o r y and t h e r e can b e s u b s t a n t i a l d i f f e r e n c e s between r e s u l t s from different laboratories. Thus, t h e r e i s a need f o r e x t e n s i v e

measurements o f t h e s c a t t e r i n g law f o r D 0 a t t h e h i g h e s t 2 p r a c t i c a l temperatures. Such e x p e r i m e n t s s h o u l d b e d e s i g n e d t o

p r o v i d e a k e r n e l f o r t h e e n t i r e r a n g e o f bound d e u t e r o n motions. C o r r e c t i o n s f o r m u l t i p l e s c a t t e r i n g and o t h e r e f f e c t s

s h o u l d , o f c o u r s e , b e made t o t h e e l e v a t e d t e m p e r a t u r e d a t a .

depends on t h e r e l a t i v e a l i g n m e n t of t h e n e u t r o n and n u c l e a r spins. For hydrogen t h e p h a s e s h i f t s a r e o f o p p o s i t e s i g n ,

with t h e f o r t u i t o u s r e s u l t t h a t coherent s c a t t e r i n g i s n o t s i g n i f i c a n t i n H20. The r e s t r i c t i o n t o i n c o h e r e n t s c a t t e r -

i n g means t h a t o n l y a d e s c r i p t i o n of t h e dynamics of s i n g l e atoms i s needed t o c a l c u l a t e t h e s c a t t e r i n g c r o s s s e c t i o n s .

(77) (As shown by Van Hove,


significant i n D 0 2

coherent s c a t t e r i n g

- which

is

depends on t h e c o r r e l a t e d dynamics of

p a i r s of atoms, and i s t h u s much more d i f f i c u l t t o c a l c u l a t e . ) A f u r t h e r s i m p l i f i c a t i o n o c c u r s i n H 0 b e c a u s e t h e hydrogen 2 c r o s s s e c t i o n i s much l a r g e r t h a n t h e oxygen c r o s s s e c t i o n , and t h u s oxygen s c a t t e r i n g can b e n e g l e c t e d o r t r e a t e d approximately. P r e s e n t models f o r D 0 u s e m o d i f i c a t i o n s of models 2 f i r s t proposed f o r H 0 , t o c a l c u l a t e t h e i n c o h e r e n t c o n t r i 2 bution t o the scattering.
2

Thus i t w i l l b e c o n v e n i e n t t o
A l l c r i t i c a l comments

b e g i n w i t h a review of H 0 k e r n e l s .

i n t h i s s e c t i o n w i l l , of c o u r s e , a p p l y e q u a l l y w e l l t o t h e i n c o h e r e n t p a r t of t h e c o r r e s p o n d i n g D 0 k e r n e l . 2 b. HOKernels 2 S e v e r a l models h a v e b e e n proposed t o d e s c r i b e t h e motion of hydrogen i n w a t e r . The e a r l i e s t s u c h model, a l s o

a p p l i e d t o o t h e r m o d e r a t o r s , assumes t h a t t h e hydrogen moves a s i n a f r e e g a s , (78) and a l l chemical b i n d i n g e f f e c t s a r e ignored. S i n c e t h i s model does n o t r e p r o d u c e

t h e measured t o t a l c r o s s s e c t i o n of H 0 , a m o d i f i c a t i o n h a s 2

b e e n s u g g e s t e d by Brown and S t . John.

The f r e e g a s

b e h a v i o r i s r e t a i n e d , b u t t h e dependence of t h e c r o s s s e c t i o n on t h e neutron-nucleus r e l a t i v e v e l o c i t y i s assumed

t o b e g i v e n by a ( n o n - p h y s i c a l ) sum of e x p o n e n t i a l s , w i t h t h e p a r a m e t e r s chosen t o f i t t h e measured t o t a l c r o s s section. While b o t h of t h e s e g a s - l i k e models have b e e n

a p p l i e d t o H 0 , t h e y a r e now g e n e r a l l y conceded t o b e 2 i n a d e q u a t e a t t h e r m a l e n e r g i e s b e c a u s e of t h e i r complete n e g l e c t o f i n t e r a c t i o n s between n e i g h b o r i n g atoms. The f i r s t model which s e r i o u s l y a t t e m p t e d t o d e s c r i b e t h e motion o f hydrogen i n w a t e r was proposed by N e l k i n (71) i n 1960. I n t h e N e l k i n model, i t i s assumed t h a t e a c h m o l e c u l e

h a s t h e same i n t e r n a l v i b r a t i o n a l modes t h a t o c c u r i n t h e vapor s t a t e . I n a d d i t i o n , i t i s assumed t h a t t h e h i n d e r e d

r o t a t i o n a l motion o f t h e e n t i r e m o l e c u l e can b e r e p r e s e n t e d a s a harmonic t o r s i o n a l o s c i l l a t i o n a t a s i n g l e f r e q u e n c y . The h i n d e r e d t r a n s l a t i o n a l motion i s assumed t o i n v o l v e o s c i l l a t i o n s a t f r e q u e n c i e s s o low t h a t n e u t r o n s c a n n o t d i s t i n g u i s h t h e m o l e c u l a r t r a n s l a t i o n s from t h o s e o f a f r e e gas. Thus t h e N e l k i n model p r o p o s e s i n e s s e n c e t h a t H 0
2

r e s e m b l e s a harmonic c r y s t a l h a v i n g a normal mode d i s t r i b u t i o n c o n s i s t i n g o n l y of d e l t a f u n c t i o n s , one a t 33w = 0 ( t r a n s l a t i o n ) , one a t 5 w


=

.06 eV ( h i n d e r e d r o t a t i o n ) , one

~ a t 5 w = 0.205 eV ( v i b r a t i o n ) , and one a t - 6 = 0.481 eV.


( r e p r e s e n t i n g t h e two c l o s e l y s p a c e d h i g h e n e r g y v i b r a t i o n a l modes). I n s p i t e o f t h e p l a n a r n a t u r e of t h e w a t e r m o l e c u l e ,

t h e N e l k i n model t r e a t s e a c h of t h e above f r e q u e n c i e s a s a symmetric harmonic o s c i l l a t o r and e v a l u a t e s t h e c r o s s s e c t i o n u s i n g t h e g e n e r a l r e s u l t of Zemach and G l a u b e r (80 f o r a s y s t e m of symmetric harmonic o s c i l l a t o r s . The a n i s o t r o p i c n a t u r e of t h e m o l e c u l a r v i b r a t i o n s i s c o n s i d e r e d i n a n e x t e n s i o n of t h e N e l k i n model p r o p o s e d by Koppel and Young (81) i n 1964. Their frequency spectrum

a l s o c o n s i s t s of f o u r d e l t a f u n c t i o n s , b u t now t h e r e l a t i v e w e i g h t s depend on t h e o r i e n t a t i o n of t h e m o l e c u l e w i t h r e s p e c t t o t h e n e u t r o n , and t h e s c a t t e r i n g c r o s s s e c t i o n i s obtained by averaging t h e r e s u l t s (numerically) over orientations. While t h i s model p r e d i c t s i n f i n i t e medium s p e c t r a

i n c l o s e r agreement w i t h e x p e r i m e n t t h a n does t h e N e l k i n model, i t h a s n o t been used w i d e l y , p r o b a b l y b e c a u s e of t h e s u b s t a n t i a l i n c r e a s e i n computation time. Finally, i t

s h o u l d b e n o t e d t h a t more r e c e n t c a l c u l a t i o n s by McMurry and R u s s e l l (65) u s i n g t h e same model g i v e somewhat d i f f e r e n t values f o r t h e t o t a l c r o s s s e c t i o n than those reported by Koppel and Young. resolved. McMurry and R u s s e l l (65) (MR) have a l s o proposed a n o t h e r e x t e n s i o n of t h e N e l k i n model. While r e t a i n i n g t h e This d i f f e r e n c e h a s n o t y e t been

a s s u m p t i o n of i s o t r o p i c harmonic v i b r a t i o n s , t h e y a d m i t t h a t t h e m o t i o n of hydrogen i n w a t e r i s t o o complex t o b e d e s c r i b e d by f o u r d i s c r e t e f r e q u e n c i e s a l o n e , and u s e a f r e q u e n c y s p e c t r u m c o n s i s t i n g of twenty d e l t a f u n c t i o n s .

They r e t a i n t h e t r a n s l a t i o n a l and v i b r a t i o n a l modes o f t h e N e l k i n model w h i l e r e p l a c i n g t h e s i n g l e h i n d e r e d r o t a t i o n a l f r e q u e n c y by s e v e n t e e n new f r e q u e n c i e s . M interpret R

t h e s e f r e q u e n c i e s a s b e i n g due t o r o t a t i o n s of b o t h f r e e m o l e c u l e s and a g g r e g a t e s of many m o l e c u l e s , and t o i n t e r n a l v i b r a t i o n s of a g g r e g a t e s of m o l e c u l e s . (While t h i s i n t e r p r e -

t a t i o n a i d s i n t h e s e l e c t i o n of t h e p a r a m e t e r s of t h e model i t does n o t seem t o b e e s s e n t i a l f o r t h e u s e o f a twenty-delta f u n c t i o n f r e q u e n c y spectrum.) For s i m p l i c i t y ,

M assume t h a t t h e a g g r e g a t e s c o n s i s t of e i t h e r 75 o r 150 R molecules.


MR r e p o r t v e r y good agreement between t h e i r

model and e x p e r i m e n t f o r t h e t o t a l c r o s s s e c t i o n , and c o n s i d e r a b l e improvement o v e r t h e N e l k i n model i n t h e a v e r a g e c o s i n e of t h e s c a t t e r i n g a n g l e . The models of N e l k i n , Koppel-Young, and MR a l l t r e a t

w a t e r a s a q u a s i - c r y s t a l l i n e s u b s t a n c e c h a r a c t e r i z e d by a frequency spectrum. T h i s i s o f c o u r s e o n l y an a p p r o x i m a t i o n

t o a r e a l l i q u i d , f o r which t h e d i s t r i b u t i o n of normal modes i s n o t even d e f i n e d . The c o n c e p t of a f r e q u e n c y

s p e c t r u m can n o n t h e l e s s b e d e f i n e d f o r a g e n e r a l dynamical s y s t e m i n terms of t h e F o u r i e r t r a n s f o r m of t h e v e l o c i t y autocorrelation function. For a s o l i d t h e f r e q u e n c y spectrum i s

i d e n t i c a l t o t h e normal mode d i s t r i b u t i o n , w h i l e f o r a l i q u i d o n l y t h e former i s d e f i n e d . For a harmonic c r y s t a l ,

t h e s c a t t e r i n g i s c o m p l e t e l y d e t e r m i n e d by t h e f r e q u e n c y spectrum p ( B ) , but f o r a l i q u i d t h i s not t h e case. An

approximate e x p r e s s i o n f o r t h e s c a t t e r i n g c r o s s s e c t i o n of a l i q u i d , i n v o l v i n g o n l y p ( B ) , can b e g i v e n and i s known a s t h e Gaussian approximation.


I t was f i r s t p r o p o s e d by

Vineyard (82) and h a s been f u r t h e r developed by E g e l s t a f f and S c h o f i e l d . (59)

A l l of t h e above models can now b e s e e n t o b e equival e n t t o t h e use of t h e Gaussian approximation w i t h t h e a c t u a l f r e q u e n c y s p e c t r u m approximated by a s e r i e s of d e l t a functions. (Even t h e i d e a l g a s model i s s u c h a n a p p r o x i -

m a t i o n w i t h t h e f r e q u e n c y s p e c t r u m r e p l a c e d by a s i n g l e d e l t a function a t zero frequency.)

A s an a l t e r n a t i v e t o s u c h

models, E g e l s t a f f and S c h o f i e l d (59) have shown how t h e a c t u a l f r e q u e n c y s p e c t r u m can b e o b t a i n e d from e x p e r i m e n t a l scattering data. I f a p r e c i s e d e t e r m i n a t i o n of p(B) w e r e

p o s s i b l e by t h i s method t h e r e would c l e a r l y b e l i t t l e f u r t h e r need f o r t h e s i m p l i f i e d models d i s c u s s e d above. However, i n p r a c t i c e c o n s i d e r a b l e c o m p l i c a t i o n s a r i s e from c o h e r e n t e f f e c t s and ( p a r t i c u l a r l y ) m u l t i p l e s c a t t e r i n g which l e a d t o l a r g e u n c e r t a i n t i e s i n t h e measured p ( 6 ) . These d i f f i c u l t i e s have n o t y e t b e e n overcome, a l t h o u g h many a p p r o x i m a t e measurements of p(B) f o r H 0 h a v e b e e n r e p o r t e d 2 i n t h e l i t e r a t u r e , t h e most r e c e n t (and presumably b e s t ) b e i n g t h o s e of Haywood (84) and H a r l i n g . ( 8 5 ) Improved t e c h n i q u e s f o r m u l t i p l e s c a t t e r i n g c o r r e c t i o n s w i l l no doubt make more p r e c i s e d e t e r m i n a t i o n s of p(B) possible i n t h e future. The e v e n t u a l l i m i t a t i o n s on t h e

(83)

a c c u r a c y of t h e s c a t t e r i n g k e r n e l s o b t a i n e d from p ( B ) w i l l t h u s depend on t h e ( p r e s e n t l y n o t w e l l known) dynamic e f f e c t s i g n o r e d by t h e G a u s s i a n a p p r o x i m a t i o n . However, a s

r e p o r t e d by Honeck (86) t h e b e s t p r e s e n t k e r n e l s a r e a l r e a d y considered t o b e adequate f o r use i n r e a c t o r design. (While

p r e s e n t i n g h i s p a p e r , Honeck remarked t h a t t h i s s t a t e m e n t was i n t e n d e d t o a p p l y t o U low-lying


235

s y s t e m s ; f o r Pu systems t h e

r e s o n a n c e n e c e s s i t a t e s a more p r e c i s e d e s c r i p t i o n

o f t h e e p i t h e r m a l s p e c t r u m , and t h u s r e q u i r e s a more sophisticated scattering kernel.) Thus, w h i l e more a c c u r a t e

d e t e r m i n a t i o n s of p ( B ) a r e c e r t i n a l y d e s i r a b l e , c o n s i d e r a t i o n of t h e more s u b t l e non-Gaussian e f f e c t s w i l l p r o b a b l y n o t b e n e c e s s a r y f o r H 0.
2

c.

D 0 Kernels 2

W have a l r e a d y remarked t h a t n e u t r o n s c a t t e r i n g by e
D 0 i s c o m p l i c a t e d by s i g n i f i c a n t c o n t r i b u t i o n s from i n t e r -

f e r e n c e s c a t t e r i n g and from s c a t t e r i n g by t h e oxygen.

In

seeming d e f i a n c e of t h e s e f a c t s , Honeck (87) h a s proposed t h a t t h e N e l k i n model, w i t h some s l i g h t m o d i f i c a t i o n s i n t h e v i b r a t i o n a l and r o t a t i o n a l f r e q u e n c i e s , b e a p p l i e d d i r e c t l y t o D20. The oxygen c o n t r i b u t i o n t o t h e t o t a l c r o s s s e c t i o n

i s t a k e n t o b e a c o n s t a n t , i n d e p e n d e n t of e n e r g y , w h i l e t h e

coherent e f f e c t s a r e neglected completely!

Honeck j u s t i f i e s

t h i s n e g l e c t by p o i n t i n g o u t t h a t P l a c z e k (88) h a s shown t h a t t h e f i r s t e n e r g y t r a n s f e r moment of t h e i n t e r f e r e n c e s c a t t e r i n g i s always z e r o , w h i l e t h e c o n t r i b u t i o n of i n t e r f e r e n c e

s c a t t e r i n g t o t h e t o t a l c r o s s s e c t i o n o s c i l l a t e s about z e r o , w i t h a s m a l l amplitude a t h i g h e r e n e r g i e s . Thus t h e e n e r g y

t r a n s f e r moments of t h e c r o s s s e c t i o n s h o u l d n o t c o n t a i n l a r g e c o n t r i b u t i o n s from i n t e r f e r e n c e s c a t t e r i n g . Honeck's

c a l c u l a t e d t o t a l c r o s s s e c t i o n i s i n d e e d i n good agreement w i t h e x p e r i m e n t f o r E > . O 1 eV, a l t h o u g h i t is h i g h by a f a c t o r of about 2 f o r E < . 0 0 1 e V . I n a d d i t i o n , Honeck

c a l c u l a t e s d i f f u s i o n and d i f f u s i o n c o o l i n g c o e f f i c i e n t s f o r
D 0 , and o b t a i n s numbers a g r e e i n g ( w i t h i n e x p e r i m e n t a l 2

a c c u r a c y ) w i t h t h e r e s u l t s of p u l s e d n e u t r o n e x p e r i m e n t s ; however, h e s p e c u l a t e s t h a t q u a n t i t i e s s e n s i t i v e t o t h e h i g h e r a n g u l a r moments of t h e c r o s s s e c t i o n w i l l n o t b e c o r r e c t l y p r e d i c t e d by h i s model. The r o l e of i n t e r f e r e n c e s c a t t e r i n g i n D 0 i s i n v e s t i -

g a t e d f u r t h e r i n t h e work of B u t l e r (75) and Koppel and Young (76)

B u t l e r assumes t h e same four-f requency dynamical

model o f t h e D 0 m o l e c u l e s u g g e s t e d by Honeck, b u t u s e s 2 t h e g e n e r a l f o r m a l i s m of Zemach and G l a u b e r b o t h t h e i n c o h e r e n t , and t h e i n t r a - m o l e c u l a r contributions t o the cross section. t h e inter-molecular t o evaluate interference

I n addition, he obtains

i n t e r f e r e n c e c o n t r i b u t i o n from a s i m p l e

model i n which atoms i n d i f f e r e n t m o l e c u l e s a r e assumed t o a p p e a r a s randomly d i s t r i b u t e d , s t a t i o n a r y h a r d s p h e r e s . T h i s model i s a d m i t t e d l y c r u d e , b u t i s p e r h a p s a l l t h a t i s w a r r a n t e d i n t h e a b s e n c e of a more d e t a i l e d knowledge of t h e i n t e r a c t i o n s and r e s u l t i n g complex, time-dependent,

31

BNWL- 1119

c o r r e l l a t e d dynamics of p a i r s of m o l e c u l e s i n a l i q u i d . The u s e o f t h e s t a t i o n a r y a p p r o x i m a t i o n does f i n d some j u s t i f i c a t i o n i n t h e e x p e r i m e n t a l o b s e r v a t i o n of Brockhouse (89) o f a peak of a p p r o x i m a t e l y e l a s t i c a l l y s c a t t e r e d n e u t r o n s i n D 0 which does n o t o c c u r i n H 0: t h e 2 2 s t a t i o n a r y a p p r o x i m a t i o n does l e a d t o an e l a s t i c peak. Some n u m e r i c a l r e s u l t s a r e g i v e n by B u t l e r t o d i s p l a y t h e r e l a t i v e c o n t r i b u t i o n s of t h e i n c o h e r e n t , and t h e i n t r a and i n t e r - m o l e c u l a r section. E x t e n s i v e c a l c u l a t i o n s b a s e d on B u t l e r ' s model a r e r e p o r t e d by Koppel and Young, (76) who a l s o c o r r e c t some n u m e r i c a l e r r o r s made i n B u t l e r ' s o r i g i n a l work. summary of t h e i r c o n c l u s i o n s w i l l b e g i v e n h e r e :
1.

interference scattering t o the cross

Only a

I n t e r f e r e n c e s c a t t e r i n g i s important primarily f o r s m a l l e n e r g y and momentum t r a n s f e r s .

2.

I n t h e t o t a l c r o s s s e c t i o n , t h e i n t r a - and i n t e r m o l e c u l a r i n t e r f e r e n c e terms a r e o f o p p o s i t e s i g n and n e a r l y cancel. Thus f o r E > .004 eV t h e t o t a l c r o s s

s e c t i o n i s w e l l - r e p r e s e n t e d by t h e i n c o h e r e n t p a r t a l o n e ( a s observed by Honeck). I f interference effects are

i n c l u d e d , t h e p r e s e n t model i s a d e q u a t e t o c a l c u l a t e t h e t o t a l c r o s s s e c t i o n down t o E
=

.002 eV.

3.

The a v e r a g e c o s i n e of t h e s c a t t e r i n g a n g l e i s w e l l r e p r e s e n t e d by t h e i n c o h e r e n t c o n t r i b u t i o n a l o n e f o r E > 0 . 1 eV; however, i n t e r f e r e n c e e f f e c t s a r e i m p o r t a n t a t lower e n e r g i e s .

4.

The angular-dependent

cross section (integrated over

e n e r g y ) shows c o n s i d e r a b l e s t r u c t u r e due t o i n t e r f e r e n c e e f f e c t s , and i s i n g e n e r a l agreement w i t h t h e e x p e r i m e n t a l r e s u l t s o b t a i n e d by S p r i n g e r (90) and by G e n e r a l Atomic. (91) The above c o n c l u s i o n s i n d i c a t e t h a t a t l e a s t i n f i n i t e medium s p e c t r a w i l l b e p r e d i c t e d a d e q u a t e l y by an i n c o h e r e n t s c a t t e r i n g model e x c e p t a t v e r y low e n e r g i e s . Thus t h e r e i s c o n s i d e r a b l e j u s t i f i c a t i o n f o r c o n s i d e r i n g improvements of t h e Honeck-Nelkin model t o b e t t e r c a l c u l a t e t h e incoherent contribution t o the cross section. R e c e n t l y , McMurry ( 7 2 ) h a s proposed t h a t a m o d i f i c a t i o n of t h e MR model b e a p p l i e d t o D20. The twenty d e l t a

f u n c t i o n s a r e r e t a i n e d , b u t t h e f r e q u e n c i e s and w e i g h t s a r e a d j u s t e d somewhat t o f i t t h e s c a t t e r i n g d a t a of Haywood (60) and t h e d o u b l e d i f f e r e n t i a l c r o s s s e c t i o n d a t a of Whitternore.(92) The f i t i s c o n s i d e r a b l y b e t t e r t h a n can b e

o b t a i n e d w i t h t h e Honeck-Nelkin model. F i n a l l y , j u s t a s i n H 0 , t h e incoherent s c a t t e r i n g can 2 b e d e s c r i b e d a p p r o x i m a t e l y i n terms of a frequency s p e c t r u m p(B) measured by e x p e r i m e n t .


While c o n t r i b u t i o n s

due t o c o h e r e n t s c a t t e r i n g , and t h e s i g n i f i c a n t oxygen c o n t r i b u t i o n , make a p r e c i s e d e t e r m i n a t i o n of p(B) even more d i f f i c u l t t h a n i n H 0 , measured frequency s p e c t r a f o r 2


D 0 have been reported i n t h e l i t e r a t u r e ( s e e e.g., 2

page(:')

Haywood and P a g e , (68) and H a r l i t ~ ~ ' f~ r ) e c e n t o~ r

33
measurements).

BNWL-1119

The paper of Haywood and Page a l s o shows

t h e c o r r e c t i o n s a p p l i e d t o t h e d a t a t o account f o r m u l t i p l e s c a t t e r i n g and s c a t t e r i n g by oxygen: t h e o v e r a l l c o r r e c t i o n


is quite significant.

d.

E v a l u a t i o n of E x i s t i n g Kernels
A s f i r s t observed by Honeck, t h e i n c o h e r e n t Honeck-

Nelkin model p r e d i c t s t h e t o t a l c r o s s s e c t i o n f o r E > . O 1 eV, a s w e l l a s d i f f u s i o n and d i f f u s i o n c o o l i n g c o e f f i c i e n t s , q u i t e well.


A s e r i e s of experiments performed a t General

~ t o m i c ( ~ ~ have ~ u' b~e c t e d t h i s model t o more s e v e r e ' ~ s j ~ ) tests. Neutron s p e c t r a have been measured i n D 0 s o l u t i o n s 2

of b o t h l / v and resonance a b s o r b e r s and t h e r e s u l t s compared t o p r e d i c t i o n s based on t h e Honeck-Nelkin model. These

experiments, which a r e summarized by McNeil, e t a l , (9 7) show t h a t except f o r E < . O 1 eV t h i s model p r e d i c t s i n f i n i t e medium s p e c t r a very c l o s e l y , w h i l e s p e c t r a measured a t t h e s u r f a c e of t h e system, where a n i s o t r o p i c e f f e c t s a r e most pronounced, a r e i n e r r o r by about 12%. p r e d i c t i o n s based on t h e Brown-St. (As a c o n t r a s t ,

John model a r e a l s o These

shown, and e x h i b i t c o n s i d e r a b l y l a r g e r e r r o r s . )

r e s u l t s a r e i n accord w i t h t h e o b s e r v a t i o n s of Koppel and Young t h a t c o h e r e n t e f f e c t s a r e s i g n i f i c a n t o n l y when t h e energy i s low o r when q u a n t i t i e s s e n s i t i v e t o t h e a n g u l a r dependence of t h e c r o s s s e c t i o n a r e considered. Both t h e MR model, i n which t h e parameters a r e s e l e c t e d t o f i t t h e double d i f f e r e n t i a l c r o s s s e c t i o n d a t a , and t h e

E g e l s t a f f - S c h o f i e l d model, i n which t h e f r e q u e n c y s p e c t r u m i s d e t e r m i n e d d i r e c t l y from t h e d a t a i t s e l f , p r o v i d e a b e t t e r r e p r e s e n t a t i o n of t h e angular-dependent cross section than Presumably s p e c t r a more

i s p o s s i b l e w i t h t h e Honeck-Nelkin model.( 7 2 ) (93)

t h e s e models would a l s o p r e d i c t space-dependent

c l o s e l y , b u t u n f o r t u n a t e l y no e x t e n s i v e c a l c u l a t i o n s h a v e y e t been reported.

A comparison of i n f i n i t e medium s p e c t r a

b a s e d on t h e Honeck-Nelkin model, and on Haywood's measured f r e q u e n c y s p e c t r u m , h a s been r e p o r t e d by G e n e r a l Atomic, (") and shows ( u n s u r p r i s i n g l y ) a n e g l i g i b l e d i f f e r e n c e
A t lower e n e r g i e s t h e p r e d i c t e d s p e c t r a I t w i l l be of considerable i n t e r e s t t o

f o r E > . O 1 eV.

d i f f e r by a b o u t 6%.

compare t h e space-dependent models.

s p e c t r a p r e d i c t e d by t h e s e two

F i n a l l y , i t is of i n t e r e s t t o a s k how s i g n i f i c a n t t h e above d i f f e r e n c e s i n c r o s s s e c t i o n s and s p e c t r a a r e t o t h e r e a c t o r d e s i g n e r who i s more i n t e r e s t e d i n q u a n t i t i e s s u c h a s r e a c t i v i t y , c o n v e r s i o n r a t i o s , and t e m p e r a t u r e coefficients.

A s t u d y of t h i s q u e s t i o n h a s b e e n r e p o r t e d by

Su i ch ( 9 9 ) who compares c a l c u l a t i o n s of t h e s e p a r a m e t e r s b a s e d on t h e Honeck-Nelkin model w i t h t h o s e b a s e d on t h e i d e a l g a s and [Link] model. While d i f f e r e n t bound-

atom models a r e n o t compared, t h e d i f f e r e n c e s would p r o b a b l y b e smaller t h a n t h o s e between t h e Honeck-Nelkin and t h e gasl i k e models. S u i c h c o n c l u d e s t h a t t h e Honeck-Nelkin model

w i l l p r o d u c e e r r o r s of a few t e n t h s of 1% n r e a c t i v i t y i n i

35

BNWL- 1119

U-D 0 and Pu-D 0 s y s t e m s , and e r r o r s of 1-2% i n c o n v e r s i o n 2 2

r a t i o s and e t a i n U-D 0 s y s t e m s . 2

Temperature c o e f f i c i e n t s

may have e r r o r s as l a r g e as 10-15%. e. Recommendations f o r F u t u r e Work Some e x t e n s i o n s o f t h e work r e p o r t e d by S u i c h would b e of i n t e r e s t . For example, t h e c a l c u l a t i o n of e t a , r e p o r t e d

f o r U-D 0 s y s t e m s , would b e e x p e c t e d t o b e somewhat more 2 s e n s i t i v e t o t h e s c a t t e r i n g k e r n e l i n Pu-D 0 s y s t e m s 2 b e c a u s e o f t h e e p i t h e r m a l r e s o n a n c e i n Pu.


I t would b e of

i n t e r e s t t o d e t e r m i n e t h e d e g r e e of s e n s i t i v i t y .

In

a d d i t i o n , i f m a t e r i a l s s u c h as g r a p h i t e o r b e r y l l i u m ( p e r h a p s r e f l e c t o r s ) were p r e s e n t i n a D 0 system, t h e r a p i d 2 v a r i a t i o n of t h e i r c r o s s s e c t i o n s n e a r t h e Bragg c u t o f f would make t h e i r t h e r m a l a v e r a g e c r o s s s e c t i o n s s e n s i t i v e t o t h e s h a p e of t h e t h e r m a l f l u x , and t h u s t o t h e s c a t t e r i n g law of D20. The d e g r e e of t h i s s e n s i t i v i t y s h o u l d b e

determined. I f e i t h e r o f t h e above q u a n t i t i e s i s found t o b e s e n s i t i v e t o d i f f e r e n c e s between bound-atom models, t h e u s e o f a model more s o p h i s t i c a t e d t h a n t h e Honeck-Nelkin model would b e i n d i c a t e d . F i n a l l y , we have n o t e d t h a t t h e d e f i c i e n c i e s of t h e Honeck-Nelkin model, and i n d e e d of any i n c o h e r e n t model, a r e most l i k e l y t o b e pronounced i n c a s e s when a n i s o t r o p i c s c a t t e r i n g is important. Thus t r a n s p o r t c a l c u l a t i o n s

s h o u l d be c a r r i e d o u t f o r t h e most compact t y p e of Pu-D 0 2

36

BNWL-1119

lattices expected to be encountered in the near future to determine whether anisotropic scattering need be considered. (An estimate to the importance of the P component to the 1 scattering cross section might be obtained by comparing calculations based on the Honeck-Nelkin model using the P
0

com-

ponent alone with calculations based on the P and P compon0 1 ents.) If the P component is found to be significant, it 1

will be necessary to determine whether a more sophisticated incoherent kernel, perhaps using the MR or an experimental frequency spectrum, is adequate, or whether a complete coherent kernel will be needed. The comparison of experimental

space-dependent spectra with the predictions of various incoherent kernels should help to decide this question, and if such calculations are not reported in the near future they should certainly be carried out. If more detailed theoretical models are indicated, several extensions should be possible: a) The measured frequency spectrum of D 0 might be sup2

plemented by a simple diffusive model of the molecular translations to determine the spectrum in the region of small frequencies, which is not accessible to measurement. b) The effects of the anisotropy of molecular vibrations might be considered in the same manner as in the KoppelYoung model for water. c ) The inter-molecular interference effects might be calculated more precisely by using the experimental

p a i r c o r r e l a t i o n function r a t h e r than t h e hard sphere model used by B u t l e r . The above e x t e n s i o n s would n o t i n v o l v e any major t h e o r e t i .

c a l problems; r a t h e r t h e primary problems a r e t h o s e of numerical analysis: how t o c a l c u l a t e t h e c r o s s s e c t i o n a c c u r a t e l y withT h i s could b e

o u t u s i n g a p r o h i b i t i v e amount of computer time.

a c h a l l e n g i n g problem a r e a , r e q u i r i n g t h e development of s o p h i s t i c a t e d approximation methods f o r v a r i o u s r a n g e s of e n e r g i e s .


D.
'

Macroscopic Reactor C a l c u l a t i o n s Thus f a r t h e review of t h e development of c a l c u l a t i o n a l methods h a s d e a l t mainly w i t h methods used t o c a l c u l a t e t h e p r o p e r t i e s of a u n i t c e l l of t h e r e a c t o r . The p h y s i c s of t h e complete r e a c t o r a r e determined

from t h e p r o p e r t i e s of t h e u n i t c e l l u s i n g one of two g e n e r a l methods, t h e homogeneous o r t h e heterogeneous method.

1. Homogeneous Methods
I n t h e homogeneous method t h e p r o p e r t i e s of t h e homogenized u n i t c e l l a r e g e n e r a l l y used i n a few-group d i f f u s i o n t h e o r y c a l culation. Many d i f f u s i o n t h e o r y codes have been developed. Basic-

a l l y , they a r e a l l s i m i l a r i n t h a t t h e y s o l v e t h e d i f f u s i o n t h e o r y e q u a t i o n s u s i n g f i n i t e - d i f f e r e n c e methods. Some d i f f e r e n c e s

between t h e v a r i o u s codes a r e t h e number of energy groups, t h e number of s p a t i a l dimensions, t h e amount of s p a t i a l d e t a i l , t h e i n c l u s i o n o r e x c l u s i o n of u p s c a t t e r i n g , and t h e number of groups f o r downscattering. The f o l l o w i n g a r e some of t h e many a v a i l a b l e d i f f u s i o n t h e o r y codes :

38

BNWL- 1119

(33) One-dimensional codes: FOG (4 gps, AI) (32) , FAIM (18 gps, AI) , HFN (20 gps, BNW) (34) 9 Two-dimensional codes : ZADOC (2 gps, Winf rith) (35) , 20-GRAND

( gps, ORNL) (36), GAMBLE (10 gps, GGA) (37) 6


PDQ (5 gps , Wes tinghouse) (38) , EXTERMINATOR (Q50 gps, O W L ) (39), 2DB (Q50 gps,

BW) . (40)
Three-dimensional codes: WHIRLAWAY (2 gp, ORNL) (41), PERIGEE (2 gp, AECL) (42) , VIRVEL (2 gp, ASEASweden) (43), PDQ7 (5 gp, Westinghouse) (38) An exact analysis of a reactor in three dimensions is in many cases prohibitively expensive, and often exceeds the capacities of existing computers. Synthesis methods have been developed which

allow a fairly inexpensive analysis of the complex three-dimensional problems. Kap lan (47) has written a report on the development of synthesis methods up to about 1965. A further review of synthesis atr' techniques is given by c r e ' ) Heterogeneous Methods In the heterogeneous method one considers each fuel assembly as a line sink and source of neutrons with parameters determined from cell calculations. Because of the very heterogeneous nature of most D 0 lattices 2 and the fact that very mixed loadings can result from on-line, bidirectional refueling or other causes, the heterogeneous methods would appear to be a particularly natural approach to these D20 in a review published in 1968.

reactor designs. There has been considerable recent interest among certain groups, especially in Europe, in the development of heterogeneous source-sink methods. However, other groups seem to feel

that since reactors have been built and can be designed without using heterogeneous methods, the need for heterogeneous methods is questionable, except for some special applications. This feeling was expressed in a summary of a panel discussion(45) concerning heterogeneous methods at the Joint International Conference on the Physics Problems in Thermal Reactor Design, held in London, June 1967. The Savannah River Laboratory has been the main U. S. proponent of heterogeneous methods, and is currently using the codes HERESY I (46) and HERESY II(~~),which respectively employ two and up to ten energy groups. Although they are useful in their present form, these codes do suffer from a number of deficiencies, such as restrictions to effectively infinite lattices or reflectors, the assumption of zero diameter fuel assemblies, and the inability to consider moderation within fuel assemblies. Another heterogeneous code, developed and being used at Chalk River, is the two-group MICRETE ( 4 8 ) code. Some of the heterogeneous methods developed and being used in Europe are as follows: Recent Swedish work on heterogeneous codes has resulted in the code DIP (49) (dipoles, two-dimensional) , with the additional options MOP (only monopoles, two-dimensional) and MOPZ (three-

dimensional).

These codes differ from the older HETERO (50) codes

in that they assume a finite radius of fuel elements and control rods. They can accommodate ten energy groups.

Swiss work in collaboration with the Swedish group has led to (51) improvements in the three-dimensional Source-Sink program SOS. An arbitrary number of energy groups and azimuthal harmonics are included. A second heterogeneous code, BARCO inserted control rods in homogenized cores. The French are using a three-dimensional heterogeneous code, ASTYANAX. ( 5 3 ) Fourier expansions with from ten to fifteen (52) , treats partially

harmonics are used to represent axial distributions. The British have developed a two-dimensional heterogeneous code PRESTO (54) and have applied it to analyses of the Steam Generating Heavy Water Reactor. This code uses a finite fuel element radius and includes dipole components of the flux. As a result of the extensive European work on heterogeneous methods, theoretical methods are in existence for removing the restrictions presently contained in the HERESY codes. However, these advanced techniques need to be imported and adapted to U. S. computing machines before they can be used here.
I

1 1 1 .

REACTOR DATA AND ANALYTICAL CORRELATIONS The adequacy of any c a l c u l a t i o n a l method, t h a t i s meant f o r c a l c u l a t i o n of r e a c t o r p h y s i c s p a r a m e t e r s , h a s t o b e t e s t e d by a p p l y i n g t h e method t o a v a r i e t y of r e a c t o r e x p e r i m e n t s . I n o r d e r t o do t h i s , one

needs t o have a v a i l a b l e a n e x t e n s i v e body of e x p e r i m e n t a l d a t a . Reactor s t u d i e s can be divided i n t o c a t e g o r i e s , according t o t h e c o m p l e x i t y of t h e physic-a1 make-up of t h e l a t t i c e . In this section 1 ) uni-

t h r e e c a t e g o r i e s a r e u s e d , which i n o r d e r of c o m p l e x i t y a r e :

form l a t t i c e s of r o d s , 2) u n i f o r m l a t t i c e s of c l u s t e r s , and 3 ) power reactors. W i n v e s t i g a t e t h e s t a t u s of e x p e r i m e n t a l d a t a and t h e e

adequacy of c a l c u l a t i o n a l methods a s t h e y a p p l y t o t h e s e t h r e e c a t e g o r i e s , by r e v i e w i n g some of t h e i m p o r t a n t r e c e n t e x p e r i m e n t a l and analytical studies.


A.

Uniform L a t t i c e s of Rods
It i s i m p o r t a n t t o b e a b l e t o a c c u r a t e l y p r e d i c t t h e p h y s i c s

c h a r a c t e r i s t i c s of s i m p l e u n i f o r m l a t t i c e s of r o d s , b e c a u s e i f t h e c a l c u l a t i o n a l methods c a n n o t a c c u r a t e l y p r e d i c t t h e c h a r a c t e r i s t i c s of s i m p l e s y s t e m s , t h e y a r e u n l i k e l y t o b e a b l e t o p r e d i c t t h e c h a r a c t e r i s t i c s of t h e more complex power r e a c t o r s .

1.

S t a t u s of E x p e r i m e n t a l S t u d i e s
A l a r g e amount of e x p e r i m e n t a l i n f o r m a t i o n h a s b e e n a v a i l -

a b l e f o r some t i m e f o r n a t u r a l uranium-D 0 l a t t i c e s . 2 t i o n was made by Honeck and d a t a e x i s t i n g then.

A compila-

randa all'^)

i n 1964 of most of t h e

A. B. Atomenergi of Sweden h a s r e c e n t l y conducted s t u d i e s

(30)

( e x p o n e n t i a l and c r i t i c a l ) of s i n g l e - r o d l a t t i c e s of UO

( n a t u r a l and s l i g h t l y e n r i c h e d ) , U02-2 a t % Pu02, o r n a t u r a l

Tho2.

Both uniform and mixed lattices were studied. The meas-

urements comprised studies of material bucklings, spectral indices, and conversion ratios as functions of fuel composition and lattice pitch. At Saclay, France, substitution experiments( ' 0 ) have been

carried out in a natural uranium metal lattice with U-Pu fuel rods containing 0.04% or 0.30% plutonium. ured as a function of lattice pitch. A series of eight clean exponential experiments(101) has recently been conducted by Brookhaven National Laboratory using fuel rods in D 2 0 Tho2-3% 233~0 2 These measurements comprised Bucklings were meas-

studies of material bucklings, dysprosium thermal disadvantage factors, ratios of epi-cadmium to sub-cadmium captures in 232~h,and ratios of fissions in 2 3 2 ~ h those in to 233u

The Massachusetts Institute of Technology group has been engaged in the Heavy Water Lattice Project. They have accumulated an impressive amount of data (lo2) on slightly enriched uranium metal lattices, as well as on oxide fuels. The quantities measured have included buckling, P ~ 625, , ~ 628, and the

modified conversion ratio. A single element method has been investigated, which combines measurements on a single fuel element with a theory which relates the behavior of the lattice of such elements to the experimentally determined behavior of the single element. A moments method (lo3) has been developed for the analysis of flux distributions in subcritical assemblies. The method can be applied successfully to very small lattices as well as to large exponential assemblies.

BNWL- 1119
2. Status of Analytical Correlations Recent analytical

correlation^(^^^'^^^),

of natural uranium

experiments, by Savannah River Laboratory and Combustion Engineering using the HAMMER (25) code indicate excellent agreement. These studies show the largest discrepancy in k is about eff 1.5% and the average slightly less than 1%. Concerning the Swedish work, material bucklings calculated(30) with the FLEF code (integral transport theory) are systematically low. There is also a clear trend with lattice pitch, the predicted reactivity getting progressively worse as the lattice pitch is decreased. The reactivity discrepancy is 1-2.5% for

the uranium systems, and somewhat larger for the plutoniumenriched systems. Calculations(106) by Brookhaven National Laboratory of

their thorium oxide-uranium oxide experiments yield values of keff which are on the average about 1.2% too low, using the

HAMMER (25) code. The reasons for the discrepancies are not
fully understood; however, the experiments may be suspect because of the high leakage. Calculated dysprosium thermal disadvantage factors are about 2% higher than the measurements; ratios of epi-cadmium to sub-cadmium captures in 2 3 2 ~ hare generally in good agreement except for the most concentrated lattice; and calculated ratios of fissions in 2 3 2 ~ hto those in 2 3 3 ~ are lower than measured values. Clean geometry-critical

experiments with this fuel would be helpful in attempting to resolve the discrepancy that exists. Application of the HAMMER (25 code to the recent Swedish experiments (30) may also be helpful

i n resolving existing discrepancies. E x i s t i n g c a l c u l a t i o n a l methods a r e i n g e n e r a l a d e q u a t e f o r n a t u r a l uranium-fueled l a t t i c e s of s i n g l e r o d s . For systems

c o n t a i n i n g f u e l s o t h e r t h a n n a t u r a l uranium d i s c r e p a n c i e s do exist. More work n e e d s t o b e done i n t h e development of c a l c u -

l a t i o n a l methods b e f o r e e x p e r i m e n t s i n u n i f o r m l a t t i c e s of r o d s become s u p e r f l u o u s .
B.

Uniform L a t t i c e s of C l u s t e r s Uniform l a t t i c e s of c l u s t e r s r e p r e s e n t t h e n e x t h i g h e r o r d e r of complexity i n r e a c t o r s t u d i e s . The most i m p o r t a n t g e o m e t r i c a l con-

f i g u r a t i o n f o r heavy w a t e r r e a c t o r s i s t h e l a t t i c e of c l u s t e r e d f u e l elements. Therefore, t h e experiments i n t h i s category provide a

more s t r i n g e n t and more r e a l i s t i c t e s t of c a l c u l a t i o n a l methods t h a n experiments w i t h s i n g l e rod l a t t i c e s . Because of t h e l a r g e number

of p o s s i b l e d e s i g n s f o r a D 0 r e a c t o r , t h e e x p e r i m e n t s w i t h u n i f o r m 2 l a t t i c e s of c l u s t e r s c o v e r a wide r a n g e of f u e l s and c o o l a n t s . 1. S t a t u s of E x p e r i m e n t a l S t u d i e s Recent P r o j e c t s . Q u i t e a l a r g e number of e x p e r i m e n t s h a v e Many

been conducted r e c e n t l y w i t h u n i f o r m l a t t i c e s of c l u s t e r s .

of t h e s e e x p e r i m e n t s were performed i n s u p p o r t of s p e c i f i c r e a c t o r projects.


e

Some of t h e s e r e c e n t p r o j e c t s a r e t h e f o l l o w i n g :

The Swedish work ( I o 7 ) a t S t u d s v i k i n s u p p o r t of t h e Marviken r e a c t o r u s i n g 31-rod c l u s t e r s of 1 . 2 % e n r i c h e d U02 and 61-rod c l u s t e r s of 1 . 8 % e n r i c h e d U02.

Swedish work ( l o 8 ) i n s u p p o r t of t h e A g e s t a r e a c t o r u s i n g 19-rod c l u s t e r s of n a t u r a l UO


2'

The experiments (log) at Winfrith, England in support of the Steam Generating Heavy Water Reactor using 74-rod clusters of several types of fuel, e.g., 1.35% enriched U02, 0.91% enriched UO with 0.25% PuO and 0.43% 2 2 enriched UO with 0.8% PuO 2 2' Experiments (o ') l at Saclay, France in support of the

EL-4 reactor using 19-rod clusters of 1.65% enriched U02 and 18-rod clusters of 1.37% enriched UO
e

2'

Experiments (1 ') 1

at CISE, Segrate, Italy in support of

the CIRENE reactor using 7-tube clusters of natural uranium metal and 19-rod clusters of natural UO
e

2'

Euratom experiments (2 ') 1

in support of the Orgel project

which include 1) experiments at Ispra, Italy with 19rod clusters of natural uranium metal, 2) experiments (113) at Chalk River in cooperation with AECL using 7-rod clusters of UC, and 3) experiments at Bologna, Italy, in cooperation with CNEN using -/-rodclusters of UC. Measurements(4 ') I with 28-rod clusters of natural

uranium at Chalk River in support of the CANDU-BLW reactor.


o

Swiss studies (5 ') I natural uranium.

with 19- and 37-rod clusters of

Thorium has received considerable attention as an important fertile material. Thorium fuels have been used in experiments were conducted

') 1 at several laboratories. Early measurements (6

at Argonne National Laboratory using thorium oxide fuel containing 2% and 4% highly enriched UO 2 (THUD fuel). More recent experi-

ments using thorium fuel clusters are the following: Brookhaven

N a t i o n a l L a b o r a t o r y h a s i n v e s t i g a t e d ('I7) Tho2-3%

31-rod c l u s t e r s of using 2;

f u e~ r o d ~; Chalk R~v e r e x p e r i m e n t s ('I8) l s o i 2

19-rod c l u s t e r s of Tho

c o n t a i n i n g 1.5% h i g h l y e n r i c h e d UO

Savannah R i v e r s t u d i e s (119) w i t h 85-rod c l u s t e r s of Thud f u e l , and of f u e l c o n t a i n i n g a t h ~ r i u m - ~r ~ t~ o of 49.03 a s p a r t a iu of t h e r e c e n t l y d i s c o n t i n u e d HWOCR p r o j e c t of t h e USAEC; and measurements (I2') a t S t u d s v i k , Sweden, i n a j o i n t N a t i o n a l
B.

Committee f o r Nuclear Energy (CNEN)-Halden P r o j e c t - A . Atomenergi P r o j e c t u s i n g 7-rod c l u s t e r s of Tho i n g 2% U 235 02. 2

f u e l contain-

P l u t o n i u m f u e l s have been s t u d i e d a t B a t t e l l e - N o r t h w e s t under t h e USAEC Plutonium U t i l i z a t i o n Program. ies(121'122y157) These s t u d -

have u t i l i z e d 19-rod c l u s t e r s of A1-1.8 w t % 2' and have b e e n concerned w i t h t h e The e x p e r i m e n t s

Pu and U02-2 w t % PuO

r e c y c l e of plutonium i n t h e r m a l r e a c t o r s .

have b e e n conducted i n s u p p o r t of t h e Plutonium R e c y c l e T e s t Reactor. Methods e v a l u a t i o n s conducted under t h e program can

b e h e l p f u l even t o t h o s e who a r e n o t s p e c i f i c a l l y i n t e r e s t e d i n p l u t o n i u m r e c y c l e s i n c e t h e y can b e h e l p f u l i n d e t e r m i n i n g t h e a b i l i t y of v a r i o u s codes t o h a n d l e p l u t o n i u m . This i s important

t o everyone working i n t h e f i e l d f o r i n e q u i l i b r i u m uranium c o r e s 50% o r more of t h e f i s s i o n s c a n o c c u r i n p l u t o n i u m t h a t h a s been produced from 2 3 8 ~ . A r e v i e w of r e a c t o r p h y s i c s d a t a a c q u i r e d from Pu-fueled e x p e r i m e n t s i s g i v e n i n R e f e r e n c e 1 5 7 . S i m u l a t e d burned-up uranium f u e l s , c o n t a i n i n g s m a l l amounts of p l u t o n i u m , h a v e b e e n used i n some s t u d i e s .
A t Savannah R i v e r

and a t Chalk R i v e r 19- and 31-rod c l u s t e r s h a v e b e e n s t u d i e d

(123,124)

47

BNWL- 1119

which c o n t a i n t h r e e d i f f e r e n t c o n c e n t r a t i o n s of p l u t o n i u m , 0.259, 0.294, and 0.340 w t % plutonium. i n s u p p o r t of t h e

A t W i n f r i t h , England, e x p e r i m e n t s

Steam G e n e r a t i n g Heavy Water R e a c t o r p r o j e c t i n c l u d e d f u e l s w i t h two c o n c e n t r a t i o n s of plutonium, 0.25 and 0.80 w t % plutonium. Scope of Experiments. I n g e n e r a l , most of t h e c l u s t e r

s t u d i e s mentioned i n t h i s s e c t i o n h a v e i n c l u d e d measurements o f b u c k l i n g and c e l l - f i n e s t r u c t u r e p a r a m e t e r s . Some of t h e s t u d i e s

have used s e v e r a l of t h e common c o o l a n t s , s u c h a s D20, H20, a i r , and v a r i o u s o r g a n i c s . There h a s b e e n a d e f i c i e n c y of e x p e r i m e n t a l d a t a concerni n g c o e f f i c i e n t s of r e a c t i v i t y , e s p e c i a l l y c o o l a n t t e m p e r a t u r e coefficients. Such i n f o r m a t i o n c a n , of c o u r s e , b e o b t a i n e d

from o p e r a t i n g power r e a c t o r s , b u t i t would b e d e s i r a b l e t o h a v e t h i s i n f o r m a t i o n from c r i t i c a l e x p e r i m e n t s . Two s p e c i f i c

c a t e g o r i e s o f t e m p e r a t u r e c o e f f i c i e n t s t h a t have s u f f e r e d from a l a c k of d a t a a r e 1 ) t e m p e r a t u r e c o e f f i c i e n t s of burned-up c o r e s , and 2) t e m p e r a t u r e c o e f f i c i e n t s of H 0-cooled heavy 2 water reactors. The W i n f r i t h s t u d i e s w i t h S H R f u e l h a v e i n c l u d e d measureGW ments of t h e c o o l a n t t e m p e r a t u r e c o e f f i c i e n t . An e a r l y Win-

f r i t h experiment (126) a t t e m p t e d t o s i m u l a t e temperature-dependent e f f e c t s by u s i n g m i x t u r e s of H 0 and D 0 t o s i m u l a t e r e d u c t i o n s 2 2 of c o o l a n t d e n s i t y . More r e c e n t e x p e r i m e n t s have b e e n

conducted i n which a S H R c e l l h a s been p r e s s u r i z e d and h e a t e d GW up t o 270C. The Savannah R i v e r L a b o r a t o r y h a s been c o n d u c t i n g temperat u r e c o e f f i c i e n t measurements u s i n g 31-rod c l u s t e r s of s i m u l a t e d burned-up f u e l . I n t h e s e e x p e r i m e n t s t h e y have used f o u r d i f The

ferent coolants t o simulate boiling l i g h t water coolant.

Savannah River measurements will provide much-needed data on reactivity coefficients of burned-up cores. The range of these temperature coefficient measurements needs to be extended to other lattice pitches and other coolants. Both the Savannah River and Winfrith temperature coefficient experiments have been conducted with H 0 coolant. The
2

cooled, D 0 moderated reactor concept is receiving consid2

erable interest. In addition to the British SGHWR, the Canadian CANDU-BLW and the Italian CIRENE Reactor (129)

represent this reactor concept. The prediction of temperature coefficients in these reactors is complicated by the fact that two very different moderators, H 0 and D 0, at different
2

temperatures, have to be considered in the cell calculation. Measurements of temperature coefficients are thus very helpful for evaluating calculational methods, and should be extended to include other fuels and other lattice pitches.

2.

Status of Analytical Correlations All of the experimental studies of cluster lattices have been accompanied by calculational studies. Some calculational

studies have been confined to the use of recipes, while other studies have included the use of more sophisticated calculational tools. Recipes. the following : The Swedish code REBUS") (an improved version of the Recent calculational studies using recipes include

early BURNUP (6) code) was applied(130) to more than 250 experimental bucklings reported from six nations. The

of a l l c a l c u l a t e d v a l u e s of k t h e experimental k eff

eff

l a y w i t h i n ? 0.5% of

'

and l e s s than 10% of t h e c a s e s

were i n disagreement by more than ? 1%. A s y s t e m a t i c u n d e r e s t i m a t i o n of k eff and k,was observed f o r 19-rod

uranium m e t a l c l u s t e r s .

It i s f e l t t h a t t h e main cause

of e r r o r s i n PINOCCHIO l i e s i n t h e c y l i n d r i c a l homogeniz a t i o n of t h e c l u s t e r f o r t h e thermal c e l l c a l c u l a t i o n . Work i s i n p r o g r e s s a t I s p r a t o a l l o w t h e e x a c t geometry of t h e c l u s t e r t o b e i n c l u d e d i n t h e thermal (THERMOS) calculations.


e

A t W i n f r i t h , b o t h t h e d e s i g n method METHUSELAH (132) and

t h e more s o p h i s t i c a t e d method WIMS (29) have been applied (109,125,127) t o s e v e r a l l a t t i c e experiments conThe r e a c t i v i t y p r e d i c t i o n s

ducted i n s u p p o r t of t h e SGHWR.

of METHUSELAH a r e s l i g h t l y b e t t e r t h a n t h o s e of WIMS, i n which t h e ring-smearing o p t i o n was used f o r t h e c l u s t e r s . However, even w i t h WM t h e worst c a s e i s o n l y 1% I S lower than experiment. f u e l s , eigenvalues With mixed PuO -UO 2 2

c a l c u l a t e d w i t h Methuselah d e c r e a s e w i t h i n c r e a s i n g 2 3 9 ~ u c o n t e n t , w h i l e WIMS produces t h e o p p o s i t e t r e n d . The

change i n v o i d c o e f f i c i e n t w i t h i n c r e a s i n g plutonium cont e n t i s p r e d i c t e d w e l l by METHUSELAH, b u t i t i s recognized t h a t t h e r e must b e compensating e r r o r s which o f f s e t t h e i n c o r r e c t p r e d i c t i o n of plutonium/uranium f i s s i o n r a t i o s . I n b o t h uranium and plutonium f u e l s , METHUSELAH o v e r - e s t i mates t h e thermal f l u x shape (peaking) a c r o s s a f u e l c l u s t e r . The r i n g - t o - r i n g d i s t r i b u t i o n of f i s s i o n s (thermal and

f a s t ) and of resonance e v e n t s a r e p r e d i c t e d b e t t e r by WM I S

51
t h a n by METHUSELAH.

B W - 1119 N L

The WIMS code h a s b e e n a p p l i e d a l s o t o I n o n l y one c a s e of 1 2 r e p o r t e d

some Canadian ZED l a t t i c e s .

i n R e f e r e n c e 132 does t h e c a l c u l a t e d e i g e n v a l u e d i f f e r from experiment by more t h a n 1 p e r c e n t . An o b s e r v a t i o n

r e g a r d i n g uranium-238 r e s o n a n c e a b s o r p t i o n h a s b e e n made by t h e W i n f r i t h group, on t h e b a s i s of t h i s and o t h e r s t u d i e s u s i n g t h e WIMS code. t o be strong evidence They s u g g e s t t h a t

"... t h e r e

appears

... t h a t

t h e uranium-238 c a p t u r e i s

o v e r e s t i m a t e d i n c o n d i t i o n s where t h e r e i s s u b s t a n t i a l s e l f s h i e l d i n g , and t h e d i s c r e p a n c y i s t h o u g h t t o b e due t o d a t a r a t h e r t h a n method of c a l c u l a t i o n . " (132) This suggestion has

generated f u r t h e r i n v e s t i g a t i o n , f o r i f , i n f a c t , t h e a c c e p t e d 2 3 8 ~ e s o n a n c e i n t e g r a l i s t o o l a r g e , t h i s would r have a n e f f e c t on a l l c a l c u l a t i o n s p e r t a i n i n g t o uranium reactors. However, no c o n v i n c i n g e x p e r i m e n t a l c r o s s s e c t i o n

d a t a have been o b t a i n e d t o s u b s t a n t i a t e t h i s c l a i m .
o

A t t h e Savannah R i v e r L a b o r a t o r y t h e HAIIMER (25) code h a s


been u s e d i n a n analysis(119) of 2 3 5 ~ 0-Tho 8 5 - r o d - c l u s t e r 2 2

e x p e r i m e n t s performed a s p a r t of t h e r e c e n t l y d i s c o n t i n u e d
HWOCR p r o j e c t of t h e USAEC.

C a l c u l a t e d and measured buck-2

l i n g s agreed t o w i t h i n

0.25 m

, which

corresponds t o

0.0075 i n km.

I n t r a c e l l a c t i v a t i o n p r o f i l e s were p r e -

d i c t e d a d e q u a t e l y i n most c a s e s ; s p e c t r a l i n d i c e s i n c o o l a n t s were o v e r e s t i m a t e d by t h e H M E c a l c u l a t i o n s ; and t h e measA MR ured resonance c a p t u r e i n 2 3 2 ~ h was 5 t o 20% h i g h e r t h a n that calculated. The one-dimensional H M E c a l c u l a t i o n A MR

was c o n s i d e r e d t o b e a d e q u a t e f o r c a l c u l a t i o n s of a s u r v e y

BNWL- 1119

nature. The HAMMER code h a s a l s o been applied(123) a t SRL t o a s e r i e s of experiments w i t h PuO /UO c l u s t e r s c o n t a i n i n g 2 2 t h r e e d i f f e r e n t c o n c e n t r a t i o n s of Pu02.

No s y s t e m a t i c

d i f f e r e n c e s between c a l c u l a t i o n and experiment due t o t y p e of c o o l a n t o r f u e l were observed. Agreement i n

g e n e r a l was good, b u t s i g n i f i c a n t d i s c r e p a n c i e s were observed i n t h e s p e c t r a l index and resonance c a p t u r e c a l c u l a t i o n s . These d i s c r e p a n c i e s were t e n t a t i v e l y a t t r i b u t e d p r i m a r i l y t o t h e u s e of a one-dimensional r i n g model f o r t h e h i g h l y heterogeneous c l u s t e r s .
a

A t Combustion Engineering, a version* of t h e HAMMER (25) code

h a s been a p p l i e d t o a n a l y z e ( l o 5 ) 1 ) a l a r g e number of Canadian ZED-2 experiments w i t h c l u s t e r s of UO 2'


U C , and U m e t a l , and

2) some SRL experiments w i t h PuO -UO c l u s t e r s . 2 2 C a l c u l a t e d e i g e n v a l u e s f o r D 0 and a i r - c o o l e d c l u s t e r s 2 a r e dependent on l a t t i c e p i t c h , whereas they a r e n o t s o f o r organic-cooled c l u s t e r s . The t r e n d w i t h l a t t i c e p i t c h

v a r i e s from about 3% lower than experiment t o 1.2% h i g h e r t h a n experiment. C a l c u l a t e d f a s t f i s s i o n and c o n v e r s i o n

r a t i o s d i f f e r from measured v a l u e s by amounts t h a t a r e dependent on l a t t i c e p i t c h , c o o l a n t , and t h e number of r o d s i n the cluster. I n t h e c a s e of Pu02-U02 l a t t i c e s , c a l c u l a t e d

e i g e n v a l u e s a r e low by 2 t o 3% and c a l c u l a t e d v a l u e s of
p 2 8 a r e high by 3 t o 10%.

The d i s c r e p a n c i e s i n p 2 8 and t h e dependence of eigenv a l u e on l a t t i c e p i t c h i n d i c a t e t h a t t h e resonance t r e a t m e n t *Early Brookhaven N a t i o n a l Laboratory v e r s i o n ,

53
of HAMMERmay b e inadequate.

BNWL- 1119

The dependence of e i g e n v a l u e

on number of rods p e r c l u s t e r i n d i c a t e s t h a t t h e onedimensional model of c l u s t e r may b e inadequate. A t Battelle-Northwest t h e c a l c u l a t i o n a l scheme THERMOS (18)H R G ( ~ ~ ) - H F has ~ ~ ) a p p l i e d t o a n a l y z e some plutoniumN ~ been f u e l e d experiments. For a two-zoned c o r e (133) of n a t u r a l UO eff
2

and A1-1.8 w/o Pu t h e c a l c u l a t e d k

i s about 1% i g h ; h

and f o r a l a t t i c e ( 1 2 1 b ) of A1-1.8 w/o Pu c l u s t e r s o n l y t h e c a l c u l a t e d keff i s about 5% h i g h ; however, t h e v a l i d i t y of one-dimensional d i f f u s i o n t h e o r y (HFN) i s q u e s t i o n a b l e i n t h e l a t t e r c a s e because t h e l o a d i n g c o n t a i n e d o n l y seven 19rod c l u s t e r s .
A t t h e p r e s e n t time a d e t a i l e d a n a l y s i s

i s underway

of experiments conducted i n t h e PRCF Batch Core loading(135)

i n s u p p o r t of a

of plutonium i n t h e PRTR u s i n g 192' The purpose of t h e a n a l y s i s

rod c l u s t e r s of KO2-2 w/o PuO

i s t o determine t h e l i m i t a t i o n s of v a r i o u s c a l c u l a t i o n a l

methods i n t h e i r a p p l i c a t i o n t o plutonium-fueled thermal r e a c t o r systems. and H H T The codes being used a r e :


HAMMER ( 2 7 )

(HRG-THERMOS-HFN).

I n a d d i t i o n t o t h e codes

H N and FLOG, which a r e c o n t a i n e d , r e s p e c t i v e l y , i n H H F T and H M E , t h e EXTERMINATOR code (two-dimensional) A MR being used f o r r e a c t o r c a l c u l a t i o n s .


A l a r g e and d i v e r s e amount of e x p e r i m e n t a l i n f o r m a t i o n e x i s t s

is

f o r uniform l a t t i c e s of c l u s t e r s i n D20 moderator.

Because much of

t h e d a t a h a s been g a t h e r e d i n s u p p o r t of s p e c i f i c r e a c t o r p r o j e c t s , most experimental programs have n o t s y s t e m a t i c a l l y covered a wide

range of variables, e.g., lattice pitch or fuel enrichment. Therefore, there are gaps in the body of experimental data that need to be filled if a systematic study of calculational methods is to be made over a wide range of variables. Some of these gaps are: tempera-

ture and void coefficients of lattices of simulated burned-up fuel; temperature and void coefficients of H 0-cooled lattices of all 2 fuels of interest; experiments in general with plutonium-containing fuels simulating highly burned-up fuel; experiments in general with actual burned-up fuel; experiments with thorium fuels. Discrepancies exist between experiment and calculation and between various calculational methods. Comparison of calculational

results is hampered by the use of different sets of basic nuclear data by different laboratories. Systematic calculations over a wide

range of lattices need to be done with several calculational methods using consistent basic data. C.

POWER REACTORS
1. Status of Experimental Work The ultimate goal of reactor physics studies is to be able to predict accurately the behavior of actual power reactors. Thus, the ultimate test of calculational methods is provided by physics data obtained from operating power reactors. Unfortunately, there is only a relatively small amount of such data available. One

reason for the deficiency of physics data from operating D 0 power 2 reactors is that there are relatively few D 0 power reactors in 2 operation. A second reason is that most power reactors have not been designed to conveniently yield physics data. Furthermore,

a problem arises because the reactor designer and the reactor

operator have different goals.

The reactor operator cannot

afford to devote as much time to physics experiments as the designer would like, and much of the physics information that has been obtained during operation has not been systematically organized and reported. Physics experiments at the time of reactor startup supply data with which to verify design calculations. These experiments, though somewhat more complex, are often not very different from zero power critical experiments with uniform lattices of clusters. Physics experiments at various stages of burnup would supply data with which to verify burnup calculations. These measurements, along with measurements of operating coefficients of the power reactor, are obtainable only from a power reactor. Recent reports of power reactor physics studies have appeared in the following compilations: Proceedings of an IAEA Panel of Fuel Burnup Prediction in Thermal Reactors, Vienna, April 1967. (137)
e

IAEA Symposium on Heavy Water Power Reactors, Vienna, September 1967. (138)

British Nuclear Energy Society Conference on Steam Generating and Other Heavy Water Reactors, London, May

European Nuclear Energy Association Seminar on Physics Measurements in Operating Power Reactors, Rome, May

The first of the above compilations contains excellent reviews of the state-of-the-technology, and sets forth some useful

56

BNWL- 1119

conclusions and recommendations. Parts of these reviews, csnclusions and recommendations are contained in this report. Experiments in the D 0-cooled, U02 (1.5% and 2% enriched) 2 fueled Carolinas Virginia Tube Reactor (CVTR) have been reported (141) by Westinghouse. This program has included measurements, at

various stages of burnup, of temperature coefficients, differential moderator worth, control rod worths, and reactivity depletion rate. Measurements were also made of xenon transients, power coefficient, decay heat, and direct deposition of fission energy in the moderator system. An experimental program of burnup physics has been con-

ducted with the second fuel charge of the Halden Heavy Boiling-Water Reactor in Norway. This fuel charge consisted of 7-rod clusters

of 1.5% enriched U02. A series of measurements including critical size determination, temperature reactivity coefficient, power void coefficient, cell parameter studies, and dynamic characteristics were conducted at zero burnup. Before final shutdown, measurements critical size, temperature

were made in the burned core of:

reactivity coefficient, and void power coefficient. The core had an estimated average burnup of 6200 MWd/tU. Spectral indices were Determi-

measured in coolant channels at various stages of burnup.

nations of isotopic compositions of burned-up fuel are being carried out in cooperation with AB Atomenergi of Sweden. Both destructive (mass spectrographic) and nondestructive (gamma scanning) analyses are being done. Pile oscillator techniques, using samples of burned fuel are being used in cooperation with AB Atomenergi to deduce changes in cross sections with exposure. The third Halden

core has been a mixture of various fuel assemblies, and has been used mainly to test these various fuels. Physics experiments have been conducted in the Agesta

Reactor, which is a pressure vessel reactor fueled with 19-rod clusters of natural UO 2' An extensive series of experiments was

performed at zero burnup, and measurements were made at several stages of burnup of excess reactivity, control rod patterns, temperature coefficient, power distribution, and activation of spectrum-sensitive foils. Determinations of isotopic compositions of burned-up fuel are being made using both destructive and nondestructive techniques.

A large-scale burnup experiment

(the Batch Core Experi-

ment) is underway in the Plutonium Recycle Test Reactor (PRTR). The basic fuel loading, which consists of 55 19-rod clusters of U02-2 w/o Pu02, will remain essentially unperturbed to the end of core reactivity lifetime, thus providing a unique set of data for use in checking methods of calculating reactivity lifetimes of reactor cores. This feature is noteworthy because results of previous experiments (e.g., in the Halden and Agesta reactors) suffered because of non-uniformities in loading patterns and frequent movement of fuel. In the current PRTR experiment the

central zone of 55 elements is surrounded by a buffer zone of similar fuel elements which separates the core from the test fuel elements on the periphery. No control rods or shim rods are

present to perturb the core because the reactor is controlled by varying the moderator height. Reactivity coefficients, the boron

concentration for the just critical situation, and the isotopic

c o n c e n t r a t i o n a s a f u n c t i o n of e x p o s u r e a r e b e i n g measured. of J a n u a r y 1969 a n a v e r a g e e x p o s u r e of 5300 MWdIMTM h a s b e e n a c h i e v e d f o r t h e 55-element c o r e . vided u s e f u l d a t a

As

E a r l i e r PRTR o p e r a t i o n h a s pro-

on changes i n i s o t o p i c c o m p o s i t i o n of Both d e s t r u c t i v e and nondes-

burned-up c l u s t e r s of A1-Pu a l l o y s .

t r u c t i v e t e c h n i q u e s a r e u s e d t o o b t a i n d a t a on i s o t o p i c compositions. In addition t o the isotopic data, effective cross section from t h e f u e l s and u s e d i n c o r r e l a D e t e r m i n a t i o n of e f f e c t i v e

r a t i o s have been deduced


tion

of c a l c u l a t i o n a l methods.

c r o s s s e c t i o n r a t i o s a l l o w s e p a r a t e e v a l u a t i o n of c e l l c a l c u l a t i o n methods and of burnup c a l c u l a t i o n t e c h n i q u e s . In addition, the

e f f e c t i v e c r o s s s e c t i o n s a r e a more s e v e r e t e s t of t h e methods t h a n i s o t o p i c c o n c e n t r a t i o n s o r r e a c t i v i t y measurements. The Canadian heavy-water-cooled NPD r e a c t o r h a s been

o p e r a t i n g w i t h a n a t u r a l uranium f u e l c h a r g e n e a r e q u i l i b r i u m burnup f o r a b i - d i r e c t i o n a l fueling cycle.


It i s a w e l l -

c o n t r o l l e d c r i t i c a l e x p e r i m e n t w i t h i r r a d i a t e d f u e l , i n which t h e i r r a d i a t i o n h i s t o r y of e a c h f u e l b u n d l e i s known. Neverthe-

less, c o m p l i c a t i o n s a r i s e i n t h e a n a l y s i s of t h i s l o a d i n g , b e c a u s e of t h e p r e s e n c e of many t y p e s of e x p e r i m e n t a l f u e l b u n d l e s . Chemi-

c a l a n a l y s e s have been performed t o d e t e r m i n e plutonium/uranium r a t i o s of burned-up f u e l , and mass s p e c t r o m e t r i c a n a l y s e s h a v e b e e n made t o d e t e r m i n e i s o t o p i c c o m p o s i t i o n s . S t a r t u p e x p e r i m e n t s from o t h e r r e a c t o r s , such a s t h e B r i t i s h S H R (148), GW t h e French EL4 (110), t h e German MZFR (14'), (150,151) and t h e some

Canadian Douglas P o i n t Candu r e a c t o r additional physics information.

, provide

These r e a c t o r s a r e a l s o s o u r c e s

for future information regarding burnup problems. An accurate knowledge of the power distribution in the reactor is essential for accurate prediction of burnup. For typical,

highly heterogeneous loadings involving mixed fuels, empty channels, etc., the precision of the knowledge of the power distribution has often been very poor. In an attempt to improve the

knowledge of power distributions, emphasis has been recently placed on extensive in-core instrumentation. Future studies in the Halden reactor will have extensive in-core instrumentation, as does the new Swedish Marviken reactor.

2. Status of Analytical Correlations


Methods used to calculate the physics behavior of D 0 power 2 reactors are basically the same as those used to calculate the behavior of zero-power critical lattices of clusters. There are

additional complications, such as the presence of control rods and other perturbations, and the effects of thermal hydraulics on the physics behavior of the reactor. A further problem in the calculation of power reactors is that of determining the burnup, i.e., the change in fuel isotopic composition as a function of irradiation. This is of utmost importance from a fuel-management and economic viewpoint. It is also important from the viewpoint of reactor behavior because many important reactor physics quantities change as a function of burnup. Calculational methods used for predicting fuel burnup can be classified, as were the calculational methods mentioned in Section 11, as 1) cell methods (or point burnup methods) or 2) macroscopic

60 methods.

BNWL- 1119

Cell methods are used to evaluate burnup within individual

fuel elements and macroscopic methods are used to perform over-all reactor calculations using the results of cell burnup calculations. The cell methods are useful in themselves for predicting changes in reaction rates and fuel composition for a cell which is typical of a given portion of the reactor core. include both recipe-type codes, e.g MELEAGER The cell codes (Sweden) and

. , REBUS'^)

(BNW), and more sophisticated codes that attempt to

take into account the geometry of the unit cell, e.g., PINOCCHIO (31) (EURATOM), METHUSELAH (Winfrith) , and FLEF (30) (Sweden). The

ultimate goal, however, of burnup calculations is to be able to predict fuel burnup over the whole reactor. The physics behavior of a power reactor presents a complex three-dimensional problem. The analysis is complicated by perturba-

tions such as control rods, and by the effects of thermal-hydraulics. The latter effects are especially important in cases where the coolant is boiling water, because boiling introduces a non-uniform distribution of voids throughout the reactor. If the void coefficient of

reactivity is appreciable, a non-uniform void distribution has an important influence on the behavior and burnup of the reactor. Thermal hydraulic eEfects are generally taken into account by coupling reactor physics codes to thermal-hydraulic codes. The widespread use of detailed three-dimensional calculations, such as the British JOSHUA scheme, or the Westinghouse TNT scheme, the French TRICYCLES (154) or PDQ-7 (38) schemes, is

limited by the very long computing times required., And in many practical cases the detail required for an accurate three-dimensional

calculation exceeds the capacity of existing computing machines. In some cases, for example, when the reactor loading contains fairly uniform zones of fuel, a two-dimensional calculation such as the British METHSELAH-ZADOC or ALMAZ

the French POUSSEY

POUSSE (154), the Oak Ridge ASSAULT

, General Atomic DDB (159)


scheme is

Westinghouse TURBO (160) , or the Swedish MABUS (' 1) 6

adequate; and if the loading consists of annular zones, a one-dimensional calculation; e.g., the Westinghouse CANDLE International SIZZLE

the Atomics
Y

, Battelle-Northwest ZODIAC-G (164) or


may be adequate.

the Combustion Engineering version of HAMMER

Synthesis techniques(1y44) can be used in some cases to obtain a fairly inexpensive analysis of the complex three-dimensional problems. An excellent review of current methods used for burnup calculations is presented in the Proceedings of an IAEA panel on Fuel Burnup in Thermal Reactors (137), held in Vienna, April 1967. Papers were presented from England, Canada, Czechslovakia, France, the United States, Belgium, Japan, Sweden, Norway, and the USSR. A review of European American Committee on Reactor Physics activities in burnup physics was also presented. The general opinion of this panel was

that the status of cell burnup codes is quite good, and that the main problem in burnup calculations is in the macroscopic calculation of the spatial flux and power distributions. Some conclusions and recommendations from the 1967 IAEA Panel, which indicate the current state-of-the-technology of physics calculations for power reactors, are:

"The degree of detail required in the mathematical models, the speed and capacity of our computing devices, and the nature of our mathematical methods are still incommensurate. It is believed that our theory and

data are adequate, but the computations required for practical, precise prediction are still very lengthy." There is a need to o "Develop reliable procedures for testing the precision and convergence of alternate mathematical techniques; o "Improve the speed and stability of convergence of methods used to predict large, loosely-coupled cores; o "Achieve some standards of characterization for heterogeneous codes;
o

"Develop improved general methods for dealing with fuel and absorber management problems;

"Develop improved methods for dealing with operational problems."

It was recommended

"That standard reactor configurations, including some for which the representation of details is important, be recommended as calibration standards, with which the existing large variety of computing codes may be compared. "

"Need for more and better instrumentation to obtain precise, detailed data on operating power reactors" was stressed, as well as the need for publication of such data.

IV. S m Y AND CONCLUSIONS


We have reviewed the status of heavy water reactor physics studies and, on the basis of this review, have indicated areas where further studies would be useful. Some of these areas are discussed below.

In the area of basic data, there is a continuing need to evaluate new measurements of cross sections and to update cross section libraries; there is a need for extensive measurements of the scattering law for D 0 2 at high temperatures; and there is a need for systematic comparisons of various scattering kernels and slowing down theories--especially as to their effect on important reactor physics parameters such as reactivity, reactivity coefficients and power distributions. Existing calculational methods are in general adequate for natural uranium-fueled lattices of single rods. For systems containing fuels other than natural uranium discrepancies do exist. More work needs to be done in the development of calculational methods before experiments in uniform lattices of rods become superfluous.

A large and diverse amount of experimental information exists for


uniform lattices of clusters in D 0 moderator.

Because much of the

data has been gathered in support of specific reactor projects, most experimental programs have not systematically covered a wide range of variables, e.g., lattice pitch or fuel enrichment. Therefore, there are gaps in the body of experimental data that need to be filled if a systematic study of calculational methods is to be made over a wide range of variables. Some of these gaps are: temperature and void

coefficients of lattices of simulated burned-up fuel; temperature and void coefficients of H 0-cooled lattices of all fuels of interest;

experiments in general with plutonium-containing fuels simulating highly

64

BNWL- 1119

burned-up fuel; experiments in general with actual burned-up fuel; experiments with thorium fuels. Discrepancies exist between experiment and calculation and between various calculational methods. Comparison of calculational results is

hampered by the use of different sets of basic nuclear data by different laboratories. Systematic calculations over a wide range of lattices need

to be done with several calculational methods using consistent basic data. The ultimate goal of reactor physics studies is to be able to predict accurately the behavior of actual power reactors. Thus, the ultimate

test of calculational methods is provided by physics data obtained from operating power reactors. There are many calculational methods available,

but unfortunately, there is only a relatively small amount of experimental data available. There is a need for more and better instrumentation to

obtain precise, detailed, physics data from operating power reactors. There is also a need for such detailed data to be published so that the many existing calculational methods can be meaningfully evaluated. It

is felt that the biggest problem in burnup calculations is in the macroscopic calculation of the complex spatial flux and power distributions. There is a need for the development of improved general methods for dealing with fuel management problems and operational problems.

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