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OPTICAL PROPERTIES
OF SURFACES
Second Edition
This page intentionally left blank
OPTICAL PROPERTIES
OF SURFACES
Second Edition

Dick Bedeaux
Institute of Chemistry, Norwegian University of Science
and Technology, Norway

Jan Vlieger
Leiderdorp, The Netherlands (retired)

Imperial College Press

Published by
Imperial College Press
57 Shelton Street
Covent Garden
London WC2H 9HE

Distributed by
World Scientific Publishing Co. Re. Ltd.
5 Toh Tuck Link, Singapore 596224
USA office: Suite 202, 1060 Main Street, River Edge, NJ 07661
UK office: 57 Shelton Street, Covent Garden, London WC2H 9HE

British Library Cataloguing-in-PublicationData

A catalogue record for this book is available from the British Library.

OPTICAL PROPERTIES OF SURFACES, SECOND EDITION

Copyright 0 2004 by Imperial College Press
All rights reserved. This book, or parts thereof, may not be reproduced in any form or by any means,
electronic or mechanical, includingphotocopying, recording or any information storage and retrieval
system now known or to be invented, without written permission from the Publisher.

For photocopying of material in this volume, please pay a copying fee through the Copyright
Clearance Center, Inc., 222 Rosewood Drive, Danvers, MA 01923, USA. In this case permission to
photocopy is not required from the publisher.

ISBN 1-86094-450-7

Printed in Singapore by World Scientific Printers (S) Pte Ltd

 PREFACE TO THE SECOND EDITION

The first edition of this monograph appeared two years ago. In this second edition we
have added a chapter on the reflection of light by a gyrotropic medium. In the literature
there are two methods to describe homogeneous gyrotropic media. These methods lead to
different reflection amplitudes of such a medium using the so-called standard boundary
conditions (Fresnel). The theory developed in the first edition of the book is shown to be
eminently useful to elucidate the origin of this difference. Gyrotropic contributions due to
the interfacial layer are also discussed.

Furthermore we added a section on self-affine surfaces in the chapter on rough surfaces.

Such surfaces are simultaneously flat and rough over the same range of lengths. They
have a well-defined roughness exponent. Reflection studies may give information about
this exponent.

We are grateful to Professor M. Osipov from the Strathclyde University, Glasgow, Scotland,
who drew our attention to the problems regarding the reflection amplitudes for gyrotropic
media and helped us to address these questions. We are also indebted to Dr. S. Gheorghiu
from the Technical University in Delft, The Netherlands, for his help with the section on
self-affine surfaces and to Dr. C. Chassagne from the Norwegian University of Science
and Technology, Trondheim, for her help with the figure in that section.

We also want to thank Caroline C. Vlieger for designing the cover of both editions of this
book.

February, 2004

Dick Bedeaux (Trondheim, Norway)

Jan Vlieger (Leiderdorp, The Netherlands)

Address for correspondence:

Dick Bedeaux, Institute of Chemistry,
Norwegian University of Science and Technology,
749 1 Trondheim, Norway.
Email: [email protected]
This page intentionally left blank
 PREFACE TO THE FIRST EDITION

The aim of the book is to present in a systematic manner the exact results the authors
obtained over the years for the description of the optical properties of thin films and
rough surfaces. This work found its origin 30 years ago in a discussion of one of us
(J.V.), during a sabbatical, with the late Professor Dr. G.D. Scott of the University of
Toronto, Canada, about the Maxwell Garnett theory. Many questions arose which
resulted in a paper by Vlieger on the reflection and transmission of light by a two-
dimensional square lattice of polarizable dipoles (Physica 64, page 63, 1973). When the
other author (D.B.) read this paper he was surprised by the efforts to describe the results
in terms of a layer of a finite thickness, using Maxwell Garnett, while the original model
had a polarizability, which was so clearly restricted to the plane of the surface. A choice
of the optical thickness in terms of the distance between the dipoles seemed to be
constructed. It appeared much more reasonable to replace a thin layer, compared to the
wavelength of the incident light, by an infinitesimally thin layer, than the other way
around. Of course the formulation of a new theory in terms of an infinitesimally thin
polarizable dipole layer, which was compatible with Maxwell’s equations, is easier said
than done. It turned out to be necessary to introduce singularities in the electric and
magnetic field at the surface in addition to the occurrence of such singularities in the
sources of these fields (Physica A 67, page 55, 1973). A general description was
developed, using constitutive coefficients, to describe the electromagnetic response of the
surface. Having thus convinced ourselves that this approach was feasible, we started to
apply these ideas to thin island films and rough surfaces.

In the treatment of surfaces a confusing element is “where to choose the precise location
of the surface”. For instance, for an island film one has two possible choices, one through
the average centre of the islands and the other on the surface of the usually flat substrate.
The constitutive coefficients depend on this choice. As the choice of this dividing surface
is only a matter of convenience in the mathematical description, it is clear that the
relevant observable properties, like for instance the ellipsometric angles, are independent
of this choice. To make this independence clear so-called “invariants” were introduced.
These invariants are appropriately chosen combinations of the constitutive coefficients
independent of the location of the dividing surface. The introduction of such invariants
was first done by Lekner, for the special case of thin stratified layers, and described in
1987 in his monograph on the “Theory of Reflection”. One of the chapters in this book
considers the case of thin stratified layers in detail and compares with Lekner‘s work.
 ...
Vlll PREFACE

When one moves a dipole from one choice of the dividing surface to another the dipole
moment remains the same. The displacement leads to a contribution to the quadrupole
moment, however. In order to properly describe the equivalence of different choices of
the dividing surface it is therefore necessary to describe the surface to quadrupolar order.
The relative importance of these quadrupolar terms is very dependent on the nature of the
surface. For highly absorbing metal island films they are not important. If the island
material is dielectric or when the surface is rough, the quadrupolar terms are found to be
very important. In the comparison with Lekner's results for thin stratified layers, these
quadrupolar terms are found to be essential.

For island films, thin compared to the wavelength of the incident light, two aspects are
found to be of importance. The first is the interaction of the islands with their image in
the substrate. The second is the interaction with the other islands, and with their images.
For the first problem the shape of the island is very important. Over the years we were
able to construct explicit solutions for spheres, truncated spheres, spheroids and truncated
spheroids. For different shapes, the same amount of island material is found to lead to
very different optical properties. This was also the reason to construct these explicit
solutions, as they give insight into which precise aspect of the shape might be responsible
for certain observed behavior. For the interaction along the surface one would expect the
correlations in the distribution to be important. This, however, turned out not to be the
case. Only for coverages larger than 50% this starts to be an issue. A square and a
triangular array lead to essentially the same properties as a random distribution for
coverages below 50%. Nevertheless the interaction with the other islands, though not
dependent on the details of the distribution, changes the polarizability of the islands
considerably.

For rough surfaces the correlations along the surface play a more essential role. The
quadrupolar contributions are crucial in this case. It was in fact in the study of the
contribution of capillary waves on fluid surfaces to the ellipsometric coefficient, that we
discovered the relevance of these quadrupolar contributions.

Over the years we had many stimulating contacts. Over a period of more than 25 years
Professor Dr. 0. Hunderi from the Norwegian University of Science and Technology,
Trondheim, Norway, has been a source of inspiration. His knowledge of the properties of
island films has been a great help. We are also indebted to Professors Dr. C.G.
Grandqvist and Dr. G.A. Niklasson from the University of Uppsala, Sweden, for many
discussions about island films. For the foundation of the use of singular fields, charge and
current densities we are grateful to Professor Dr. A.M. Albano from Bryn Mawr College,
Penn., USA. We had a very rewarding collaboration with Dr. R. Greef from the
University of Southampton, UK, on the optical properties of films sparsely seeded with
spherical islands with a size comparable to the wavelength. Though this subject is not
covered in this book, it added much to our understanding of the subject.
PREFACE 1x

In the past decade we had an active collaboration with the group of Professor Dr. P.
Schaaf and Dr. E.K. Mann from the Institute Charles Sadron, Strasbourg, France, and
with Dr. G.J.M. Koper of our own institution. Our insight in the use and the practical
relevance of invariants gained immensely due to this work.

Over the years we had many graduate students who contributed to the contents of this
book. In chronological order we have: Dr. B.J.A. Zielinska, Dr. M.M. Wind, Dr. P.A.
Bobbert, Dr. E.M. Blokhuis, Dr. M. Haarmans, Dr. E.A. van der Zeeuw and R. van
Duijvenbode. In particular the theoretical work of Wind and Bobbert led to significant
progress for the foundation of the whole methodology.

Recently I. Simonsen from the Norwegian University of Science and Technology,

Trondheim, Norway, ([email protected]), wrote software to perform the
calculations outlined in chapters 4-10. These progkmls have been put into operation
together with R. Lazzari from the CEA Grenoble, France ([email protected])
and it is now possible to make practical use of the analytical results in these chapters, see
http://www.phys.ntnu.no/-ingves/Software/GranularFilm/.We are very grateful to both
of them for this and for many clarifying discussions. About 60 YOof the figures in this
book were made by Lazzari who thereby contributed greatly to the usefulness and the
clarity of the sections on island films with applications. The software is available for use.
For this purpose one should consult the above mentioned web site and in case of
difficulties contact either Simonsen or Lazzari. For the other figures we are grateful to J.
van der Ploeg from our group and to L. Nummedal from the Norwegian University of
Science and Technology, Trondheim, Norway. Nummedal was also, on many occasions,
a great help solving the various software problems.

Leiden, February, 2001

Dick Bedeaux
Jan Vlieger

Address for correspondence:

Dick Bedeaux, Leiden Institute of Chemistry, Leiden University
P.O. Box 9502,2300 RA Leiden, The Netherlands
Email: [email protected]
This page intentionally left blank
 CONTENTS
PREFACE TO THE SECOND EDITION V

PWFACE TO THE FIRST EDITION vii

1 INTRODUCTION 1

2 EXCESS CURRENTS, CHARGE DENSITIES AND FIELD 7

2.1 Introduction.. ..................................... .. . ......................... ... .. 7
2.2 Excess electric current, charge density and electric field in a
conducting layer.. ......... . .. . ... ...... ..................... .. . .. . . . . :. . .......... 8
2.3 Excess electric and displacement fields in a dielectric layer.. ....... ... .... 11
2.4 Excess currents, charge density and field and the boundary conditions ... 13
2.5 Higher order moments of the excess currents, charge density and fields... 17
2.6 Boundary conditions in terms of the surface polarization and
magnetization ... ............ ... ........ ... ............... .... ......... .... . ........ 18

3 MAXWELL'S EQUATIONS WITH SINGULAR FIELDS 21

3.1 Introduction '. ... ..... .. . . ...... ..... . .. 21
3.2 Singularities in the fields, currents and charge densities 22
3.3 Maxwell's equations for singular fields and the boundary conditions ..... 23
3.4 Charge conservation ............ ... .................................. . . ........... 26
3.5 Generalized electric displacement field ..............,............,..........,. 27
3.6 Constitutive relations for isotropic interfaces without dispersion ......... 29
3.7 Constitutive relations for isotropic interfaces with spatial dispersion ..... 31
3.8 Dependence of the constitutive coefficients on the location of the
dividing surface ........................... .. . ......... .. . ................. . ... .... 33
3.9 Invariants ........................................................................... 35
3.10 Shifting the dividing surface for a film embedded in a homogeneous
medium ................. . ... ........................................................ 37
3.1 1 Superposition of adjacent films .......... . 38
3.12 Appendix A ........ .... . . ..... ...... ................ ... ........ .... . . . ...... . . ...... 41

4 REFLECTION AND TRANSMISSION 45

4.1 Introduction ........................................................................ 45
4.2 TE-waves ........................................................................... 47
4.3 TM-waves .......................................................................... 54
4.4 Reflectance and transmittance in non-magnetic systems .................... 57
xii CONTENTS

4.5 Reflectance and transmittance in non-magnetic systems at normal

incidence ........................................................................... 62
4.6 Reflectance of p-polarized light in nonmagnetic systems near the
Brewster angle .................................................................... 63
4.7 Reflectometry around an angle of incidence of 45 degrees ............... 66
4.8 Ellipsometry ...................................................................... 67
4.9 Total reflection ................................................................... 69

5 ISLAND FILMS IN THE LOW COVERAGE LIMIT 73

5.1 Introduction ....................................................................... 73
5.2 Linear response of an island .................................................... 75
5.3 Gamma and beta in the polarizable dipole model ............................ 79
5.4 Delta and tau in the polarizable dipole model ...................... 82
5.5 Polarizable quadrupole model ............. ........................ 84
5.6 Spherical islands ............................. ........................ 89
5.7 Application: Spherical gold islands on sapphire ............................. 99
5.8 Appendix A ...................................................................... 106
5.9 Appendix B ................. 115

6 SPHEROIDAL ISLAND FILMS IN THE LOW COVERAGE LIMIT 117

6.1 Introduction ...................................................................... 117
6.2 Oblate spheroids; the polarizable quadrupole model ....................... 118
6.3 Prolate spheroids; the polarizable quadrupole model ....................... 128
6.4 Oblate spheroids; spheroidal multipole expansions ........................ 137
6.5 Prolate spheroids; spheroidal multipole expansions ........................ 148
6.6 Application: Spheroidal gold islands on sapphire .......................... 156
6.7 AppendixA ............................................ ...... 165
7 ISLANDS FILMS FOR A FINITE COVERAGE 173
7.1 Introduction ...................................................................... 173
7.2 Two-dimensional arrays of sphere ............................................ 174
7.3 Regular arrays of spheres ...................................................... 177
7.4 Random arrays of spheres ...................................................... 179
7.5 Dipole approximation for spheres ..... 181
7.6 Quadrupole approximation for spheres 183
7.7 Two-dimensional arrays of spheroids . 186
7.8 Dipole approximation for spheroids ......................................... 192
7.9 Quadrupole approximation for spheroids ................................ 195
7.10 Application: Gold islands on sapphire ....................................... 201
7.1 1 Appendix A: Lattice sums ............................ .................. 214
7.12 Appendix B ...................................................................... 217

8 FILMS OF TRUNCATED SPHERES FOR A LOW COVERAGE 225

8.1 Introduction ..................................................................... 225
8.2 Truncated spheres on a substrate ............................................. 226
 ...
CONTENTS XI11

8.3 Spherical caps on a substrate .................................................. 234

8.4 Spheres and hemispheres on a substrate ..................................... 241
8.5 Thin spherical caps ............................................................. 246
8.6 Application to truncated gold spheres and caps on sapphire .............. 251
8.7 Appendix A ...................................................................... 261
8.8 Appendix B ...................................................................... 264

9 FILMS OF TRUNCATED SPHEROIDS IN THE LOW COVER-

AGE LIMIT 267
9.1 Introduction ...................................................................... 267
9.2 Truncated oblate spheroids on a substrate .................................. 268
9.3 Truncated prolate spheroids on a substrate .................................. 278
9.4 Oblate spheroidal caps on a substrate ....................................... 284
9.5 Prolate spheroidal caps on a substrate ....................................... 292
9.6 Spheroids and hemispheroids on a substrate ................................ 297
9.7 Application: Truncated gold spheroids and caps on sapphire ............ 305
9.8 Appendix A ...................................................................... 314
9.9 Appendix B ...................................................................... 318

10 FILMS OF TRUNCATED SPHERES OR SPHEROIDS FOR FINITE

COVERAGE 32 1
10.1 Introduction ...................................................................... 321
10.2 Two-dimensional arrays of truncted spherical or spheroidal islands ..... 322
10.3 Two-dimensional arrays of spherical or spheroidal caps ..................326
10.4 Dipole approximation ........................................................... 329
10.5 Quadrupole approximation ..................................................... 332
10.6 Application: Gold islands on sapphire ........................................ 336
10.7 Appendix A: Truncated particles ............................................... 355
10.8 Appendix B: Caps ................................................................ 364

I1 STRATIFIED LAYERS 371

1 1.1 Introduction ...................................................................... 371
11.2 Constitutive coefficients ....................................................... 371
11.3 Invariants ........................................................................ 373
11.4 Non-magnetic stratified layers ................................................ 375
11.5 Conclusions ...................................................................... 377

12 THE WAVE EQUATION AND ITS GENERAL SOLUTION 379

12.1 Introduction ...................................................................... 379
12.2 The wave equations ............................................................. 379
12.3 The solution of the wave equations ........................................... 381
12.4 The fields due to the surface polarization and magnetization densities ... 391
12.5 Dipole-dipole interaction along the surface .................................. 392
12.6 Appendix A ....................................................................... 394
xiv CONTENTS

13 GENERAL LINEAR RESPONSE THEORY FOR SURFACES 395

13.1 Introduction ...................................................................... 395
13.2 Green functions .................................................................. 397

14 SURFACE ROUGHNESS 401

14.1 Introduction ...................................................................... 401
14.2 General theory ................................................................... 403
14.3 Rough surfaces .................................................................. 410
14.4 Capillary waves ................................................. :............... 413
14.5 Self-affine surfaces ............................................................. 416
14.6 Intrinsic profile contributions ................................................. 418
14.7 Oxide layers ..................................................................... 420
14.8 Thin spherical caps on a substrate ............................................ 424

15 REFLECTION OF A GYROTROPIC MEDIUM 431

15.1 Introduction ..................................................................... 431
15.2 The relation between the two methods ...................................... 433
15.3 Constitutive equations ......................................................... 435
15.4 General theory .................................................................. 436
15.5 Reflection at normal incidence ................................................ 441

REFERENCES 445

INDEX 449
 Chapter 1
INTRODUCTION

It‘ is the aim of this book to describe the optical properties of surfaces with a thickness
small compared to the wavelength of the incident light. The emphasis will be on two
kinds of surfaces. The first kind consists of a film of discrete islands, small compared
to the wavelength, attached to a flat substrate. An important example of such films
are metallic films. The second kind is the rough surface. In that case the surface
resembles a landscape with hills and valleys. The height is again small compared to
the wavelength of the light. In the second edition a chapter has been added on the
reflection from a gyrotropic medium.
Historically the first description of metallic films was given by Maxwell Garnett
in 1904[1]. He developed a theory for metallic glasses, assuming the metal to be
distributed in the form of small spherical islands. The polarizability of such an island
may be shown to be equal to
E - E,
=~xE,R~-
QI
t +2ta
where E , is the dielectric constant of the glass, E the complex frequency dependent
dielectric “constant” of the metal, and R the radius of the sphere. Using the Lorentz-
Lorenz formula one then finds for the effective complex frequency dependent dielectric
constant of the metallic glass the following formula

where 4 is the volume fraction of the spheres. This formula is successful, in that it
explains for instance the striking colors of the metallic glass and their dependence on
the volume fraction. In the same paper Maxwell Garnett also applied his theory to
metallic films. In that case the islands are on the surface of the glass and surrounded
by the ambient with a dielectric constant 6,. The volume fraction is a parameter
which is not systematically defined. In practice one fits it to the experimental data,
like for instance to the minimum in the transmission, and interprets it as the weight
thickness divided by the so-called optical thickness. The experiment in this way
measures the optical thickness of the film.
Even though the Maxwell Garnett theory is very useful to describe the qual-
itative behavior of thin metallic films,the quantitative agreement is not very sat-
isfactory. One has tried to improve this along various lines. One observation is
that Lorentz-Lorenz is not adequate. An alternative popular choice for the effective
2 INTRODUCTION

dielectric constant is given, for instance, by the symmetric Bruggeman formula[2],[3]

One may show that this expression reduces to Maxwell Garnett for small volume
fractions. For a history and a description of alternative effective medium theories one
is referred to Landauer [4]. It is not our aim to discuss the various methods to make
effective medium theories work. For this we refer to various reviews, [5], [6], [7], [8]
and [9].
There are two major reasons why effective medium theories are only qual-
itatively correct for surfaces. The first reason is that the direct electromagnetic
interaction between the islands along the surface is taken into account using some 1 e
cal field argument. The choice of this local field is appropriate for a three dimensional
distribution of islands, as for instance in a metallic glass, but not for a two dimen-
sional array. The second reason is that all these theories neglect the electromagnetic
interaction with the substrate. The electric field due to the images of the spheres is
not taken into account. These images cause the polarizability of the spheres to be
different in the directions along and normal to the surface. The surface breaks the
symmetry. A dipolar model for this effect was first given by Yamaguchi, Yoshida and
Kinbara [lo].
In this book a theory for thin island films and rough surfaces is given, which
describes both the direct electromagnetic interaction along the surface and the inter-
action with the substrate. The electromagnetic properties of the surface are described
in terms of four susceptibilities, y, p, T and 6.The first coefficient y gives the inte-
grated surface polarization parallel to the surface in terms of the electric field along
the surface. The second coefficient p gives the integrated surface polarization normal
to the surface in terms of the electric displacement field normal to the surface. The
third and the fourth coefficients r and 6 are of quadrupolar order. They are not
very important for the description of metallic films,where y and p dominate the
behavior. For rough surfaces, but also for films of latex spheres on a glass substrate,
these quadrupolar terms are found to be needed, however. The book discusses the
general case for which also the integrated surface magnetization is taken along. For
the details of this aspect, which requires the introduction of magnetic analogs of the
above susceptibilities, we refer to the main text. The work described was done over
many years in our group in Leiden and will be referred to when used in the text.
For thin island films the analysis in this book is based on the calculation
of the polarizabilities of the islands. The surface is assumed to be isotropic for
translation along the surface and rotation around a normal. All islands are therefore
(statistically) equivalent. Effects due to electromagnetic interaction between islands
are calculated assuming the islands to be identical. Both regular arrays and random
arrays of islands are considered. The analysis to dipolar order gives the (average)
polarizabilities parallel, q ,and normal, a ~to,the surface per island. The resulting
dipolar susceptibilities are
INTRODUCTION 3

where p is the number of islands per unit of surface area. The (average) quadrupole
polarizabilities parallel, aho,and normal, a:', to the surface per island give the dipole
moment of the island in the direction parallel to the surface in terms of the parallel
derivative of the electric field along the surface, and the dipole moment of the island
in the direction normal to the surface in terms of the normal derivative of the electric
field normal to the surface, respectively. The resulting susceptibilities are

r = -pa;Io and 6 = - p [ a i o + LY;I~]/E,

See chapter 5 for a discussion of the definition of the polarizabilities and their relation
to the susceptibilities in the small p case. Chapters 5-10 give the explicit calculation
of dipole and quadrupole polarizabilities for spheres, spheroids, truncated spheres
and truncated spheroids on a substrate, both for small and finite p.
One may substitute the polarizabilities of the sphere surrounded by the am-
bient into eq.(1.4). This gives
& - E, € - &,
y = &3 = p a = 47rc,R3p- = 3t,Ea-
E + 2t, E + 2€,
where the weight thickness was identified with t, = 47rR3p/3. In the calculation of the
integrated excess quadrupole moments one must specify the location of the surface,
on which one locates this dipole moment. The natural choice for this dividing surface
is the surface of the substrate. Shifting the dipoles from the center of the spheres to
the surface of the substrate leads to quadrupole polarizabilities given by

Substituting this equation, together with eq.(l.l) for the polarizability, into eq.(1.5)
then gives, with eq.(1.6),

It should be noted that the quadrupole moment, due to a constant field, can be
identified with the dipole moment, due to a gradient field, on thk basis of symme
try considerations, cf. chapter 5. All interactions between the spheres have been
neglected. The above expressions are therefore only correct in the low coverage, i.e.
low weight thickness regime. Also they assume that the interaction with the image
charges in the substrate is unimportant. This is only correct if the difference between
the dielectric constants of the ambient and the substrate is negligible.
In order to compare with the Maxwell Garnett or the Bruggeman theory, one
must calculate the susceptibilities for a thin layer with a dielectric constant E e f j and
a thickness tqt. In chapter 11 the expressions for the susceptibilities of a stratified
medium are derived. Applying these expressions to a thin layer one finds
4 INTRODUCTION

Substituting the Maxwell Garnett equation, (1.2) with 4 = tw/topt,

one finds for y
and B

y = t W ( E - E,)
[ +-(
1
3:, 29
1- - ( E - E,)
1-l

(1.10)

For a small weight thickness these expressions reduce to eq.(1.6) as expected. For
larger weight thicknesses the usual depolarization factor of 1/3 for a sphere is replaced
5
by (1- tw/topt) +
along the surface and by f (1 2tw/topt) normal to the surface. The
sum of the depolarization factors over three directions remains one. This modification
is due to the electromagnetic interaction between the spheres along the surface. In
the Maxwell Garnett (LorentzLorenz) theory this is accounted for by distinguishing
between the incident field and the local field in which the dipole is placed. As he uses
a local field appropriate for a three-dimensional distribution of spheres the result is
inadequate. The formulae for 7 and 6 analogous to those given in eq.(l.lO) for y and
p may similarly be given.
The way to improve these effective medium theories is to calculate the polariz-
ability of the islands with the full electromagnetic interaction with other islands and
their images. This is the subject of chapters 5 through 10 in this book.
If one describes a surface as a 2-dimensional transition layer between the am-
bient and the substrate, as is done in this book, one needs to position this surface
at some convenient location. For the island films there are 2 natural choices. The
first is the surface of the substrate. The second is a plane through the (average)
center of the islands. The first choice, used above, makes it necessary to shift the
dipole in the center of the islands to the surface of the substrate and as a consequence
one needs to introduce multipoles, to the order of approximation in size over wav+
length one wants to describe. The second choice makes it necessary to extend the
substrate material to the center of the islands. Both choices lead to different surface
susceptibilities. In view of the fact that the experimental results are independent of
the choice of this dividing surface, they can only depend on combinations of these
susceptibilities, which do not depend on this choice. Such combinations are called
invariants. This book contains an extensive discussion of these invariants. All mea-
surable quantities, discussed in particular in chapter 4 in this book, are furthermore
given in terms of these invariants. For the special case of stratified surface layers,
such invariants were introduced by Lekner 1111. This case, and an extension thereof
to magnetic stratification, is discussed in chapter 11.
The second chapter is meant as a introduction to the use of excess electre-
magnetic fields, electric current densities and charge densities. This is done using
a number of simple examples. The aim of this chapter is to prepare the reader for
the third chapter, where the validity of the Maxwell equations is extended to electre
magnetic fields, electric current densities and charge densities, which are generalized
functions. For the last three chapters on the wave equation and its general solu-
tion, general linear response theory and surface roughness, this extension is crucial.
INTRODUCTION 5

Much of the results in these chapters could not easily be obtained without the use
of generalized functions. The general solution of the wave equation, including the
surface, is used in the chapter about linear response theory to verify that the consti-
tutive relations, given in chapter 3, are the only correct choice in view of the source
observer symmetry [12]. The general solution is used in the chapter 14 on surface
roughness to obtain contributions, due to correlations along the surface, to the surface
susceptibilities.
At the end of the second edition a chapter on the reflection of a gyrotropic
medium has been added. There are two generally accepted methods to describe the
gyrotropic nature of a homogeneous phase. Surprisingly enough these two methods
lead to different reflection amplitudes, when one uses the so-called standard boundary
conditions (Fresnel). The origin of this dflerence is discussed from the point of view
developed in this book. Additional modifications of the reflection amplitudes, due to
the possible gyrotropic nature of the interfacial layer, are discussed.
The book uses the somewhat old fashioned c.g.s. system of units rather than
the now generally accepted SI units. The reason for this is that in the c.g.s. unit
system, for instance, the electric fields, the displacement fields and the polarization
densities all have the same dimension, while they do not have this in SI units. In the
algebra using the fields one must work with similarly dimensioned fields. While this is
natural in c.g.s. units it is not in SI units. Of course one may use SI units and correct
this by adding the appropriate power of the dielectric and magnetic permittivities
of vacuum everywhere. We choose not to do this. In the experimentally relevant
formulae we have always used forms such that the unit system does not matter.
Nevertheless one should be careful regarding this point when applying the needed
formulae.
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