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The Theory of Intermolecular Forces
This page intentionally left blank
The Theory of Intermolecular Forces

Second Edition

Anthony J. Stone
University of Cambridge

1
 3
Great Clarendon Street, Oxford, ox2 6dp,
United Kingdom
Oxford University Press is a department of the University of Oxford.
It furthers the University’s objective of excellence in research, scholarship,
and education by publishing worldwide. Oxford is a registered trade mark of
Oxford University Press in the UK and in certain other countries
© Anthony J. Stone 2013
The moral rights of the author have been asserted
First Edition published in 1996
Second Edition published in 2013
Impression: 1
All rights reserved. No part of this publication may be reproduced, stored in
a retrieval system, or transmitted, in any form or by any means, without the
prior permission in writing of Oxford University Press, or as expressly permitted
by law, by licence or under terms agreed with the appropriate reprographics
rights organization. Enquiries concerning reproduction outside the scope of the
above should be sent to the Rights Department, Oxford University Press, at the
address above
You must not circulate this work in any other form
and you must impose this same condition on any acquirer
British Library Cataloguing in Publication Data
Data available
ISBN 978–0–19–967239–4
Printed and bound by
CPI Group (UK) Ltd, Croydon, CR0 4YY
Links to third party websites are provided by Oxford in good faith and
for information only. Oxford disclaims any responsibility for the materials
contained in any third party website referenced in this work.
To Sybil
Preface

The last two decades have seen considerable advances in the understanding of intermolecular
forces, in the computational methods used to calculate them, and in the experimental methods
used to investigate them. At the time of the first edition, the balance was already shifting from
experiment to computation as the prime source of information about intermolecular forces,
and this shift has continued. Experiment will continue to have an essential role, but its task
now is more to check the validity of calculations and to refine calculated potentials, rather
than to provide the principal source of data for them. Density Functional Theory has emerged
as a practical tool both for supermolecule calculations, when supplemented by an empirical
dispersion term, and as a basis for perturbation theory. It has become possible to calculate
interactions between molecules of 20 or 30 atoms to good accuracy, and methods are being
developed to describe larger molecules, for example to build proteins from an understanding
of their component amino acids. The main changes in this new edition concern these devel-
opments. Some issues that were controversial in the 1990s have been resolved and no longer
need detailed discussion, and some methods have been superseded and have been mentioned
more briefly or omitted.
My own understanding has benefited greatly from several years’ enjoyable and fruitful
collaboration with Dr Alston Misquitta, and I am glad to be able to acknowledge his consid-
erable contribution. I am indebted both to him and to Professor Sally Price for reading and
commenting on drafts of this new edition.
The book is intended to be self-contained as far as the theory of intermolecular forces
is concerned. It does assume a sound background in physics, chemistry and mathematics,
and in particular in quantum mechanics, but appendices are provided to introduce some of
the mathematical techniques. The level of the book is appropriate for graduate students and
advanced undergraduates, but it should also be useful for more experienced research workers
who require an introduction to the field.
While I have tried to ensure that this edition is free from errors, it is possible that some
will have crept through. Any that are found will be reported on my website at http://www-
stone.ch.cam.ac.uk/timf.html.
Cambridge A. J. S.
June 2012

Preface to the first edition

There have been many developments in the theory of intermolecular forces over the last twenty
years or so that have not so far been collected together in book form. After many years of
effort, practical methods have emerged for the accurate calculation of intermolecular interac-
tions by perturbation theory. Increasing computer power is making it possible to pension off
the Lennard-Jones potential after 75 years of valuable service and to use more realistic mod-
 Preface vii

els; similarly point-charge models are giving way to more sophisticated multipole descrip-
tions. This has come at a time when experimental methods for determining intermolecular
potentials are becoming more and more powerful and reliable, and when interest in accu-
rate models of intermolecular interactions is greater than ever before, not least because of the
increasing use of computer modelling for simulating systems of biological interest and for
designing biologically active molecules for use as drugs and pesticides and the like.
However, these more elaborate descriptions call for corresponding developments in the
formalism. The mathematical expressions for interaction energies involving electrostatic mul-
tipoles, for instance, are daunting for the beginner, but they can be expressed in a relatively
simple form with appropriate mathematical techniques. Forces and torques arising from these
interactions can also be manipulated much more easily than is often supposed. I have been
interested in these techniques for some time, and I have attempted in this book to set them
out in a coherent fashion. The calculation of intermolecular interactions ab initio and the con-
struction of accurate potential models are closely related topics that I have described in some
detail. The determination of intermolecular potentials from experiment, on the other hand, is
not an issue that I have attempted to cover in detail, and I have given only an outline of this
aspect of the subject to put the theory in context, together with references to fuller accounts.
It is a pleasure to acknowledge the contributions of my research students and post-doctoral
research assistants to the ideas described here, especially those of Sally Price and David Wales,
with whom I have had many stimulating discussions and rewarding collaborations in recent
years. I thank all my colleagues in the theoretical chemistry group at Cambridge for their
support and encouragement; many of them have read parts of the text in draft and made many
helpful suggestions. David Buckingham, Nicholas Handy, Ruth Lynden-Bell, David Clary
and Roger Amos have all been most agreeable and stimulating people to work with. It is a
particular pleasure, as he approaches retirement, to acknowledge the enormous contribution
made by David Buckingham to the study of molecular properties and intermolecular forces.
I am grateful also to Paul Hoang and Claude Girardet for their hospitality at the Université
de Franche Comté in Besançon, where I was Visiting Professor for a time in 1993 and where
the first draft of this book was written. I thank Bill Meath for much valuable advice and for
permission to reproduce Fig. 8.2. Many others have contributed in various ways; it would be
invidious to name a few and impossible to list everyone, but I am grateful to all of them. It
goes without saying, but it must be said, that all errors that remain are my responsibility alone.
This book was prepared using LATEX and BibTEX with the natbib bibliography package,
makeindex and hyperref. I am glad to acknowledge the generosity of the TEX community
worldwide in making their programs freely available to all.
Cambridge A. J. S.
December 1995
This page intentionally left blank
Contents

1 Introduction 1
1.1 The evidence for intermolecular forces 1
1.2 Classification of intermolecular forces 4
1.3 Potential energy surfaces 6
1.4 Coordinate systems 8
2 Molecules in Electric Fields 13
2.1 Molecular properties: multipole moments 13
2.2 The energy of a molecule in a non-uniform electric field 21
2.3 Polarizabilities 24
2.4 Hyperpolarizabilities 30
2.5 The response to oscillating electric fields 31
2.6 Symmetry properties of multipole moments and polarizabilities 34
2.7 Change of origin 39
3 Electrostatic Interactions between Molecules 43
3.1 The electric field of a molecule 43
3.2 Multipole expansion in cartesian form 45
3.3 Spherical tensor formulation 47
3.4 Examples 52
4 Perturbation Theory of Intermolecular Forces at Long Range 57
4.1 Introduction 57
4.2 The induction energy 59
4.3 The dispersion energy 64
5 Ab Initio Methods 74
5.1 Introduction 74
5.2 Electron correlation 75
5.3 Density functional theory 78
5.4 Basis sets 79
5.5 Calculation of molecular properties 83
5.6 The supermolecule method 87
5.7 Density functional theory for interaction energies 92
5.8 Semi-empirical methods 95
5.9 Potential energy surfaces 95
5.10 Energy decomposition analysis 96
6 Perturbation Theory of Intermolecular Forces at Short Range 100
6.1 Introduction 100
6.2 Symmetric perturbation methods 106
x Contents

6.3 Symmetry-adapted perturbation theories 110

6.4 The SAPT method 117
7 Distributed Multipole Expansions 122
7.1 Convergence of the multipole expansion 122
7.2 Distributed multipole expansions 123
7.3 Distributed multipole analysis 124
7.4 Other distributed-multipole methods 128
7.5 Simplified distributed multipole descriptions 130
7.6 Examples 131
7.7 Symmetry and distributed multipoles 135
7.8 Point-charge models 136
8 Short-Range Effects 141
8.1 The electrostatic energy at short range: charge penetration 141
8.2 The exchange–repulsion energy 146
8.3 The second-order energy at short range 147
8.4 The hydrogen bond 153
8.5 Halogen bonds 157
9 Distributed Polarizabilities 159
9.1 The Applequist model 161
9.2 Distributed polarizabilities 166
9.3 Computation of distributed polarizabilities 170
9.4 The induction energy in a distributed polarizability description 176
9.5 Distributed dispersion interactions 179
10 Many-body Effects 182
10.1 Non-additivity of the induction energy 182
10.2 Many-body terms in the dispersion energy 187
10.3 Many-body terms in the repulsion energy 190
10.4 Other many-body effects 190
10.5 Intermolecular forces in a medium 191
11 Interactions Involving Excited States 194
11.1 Resonance interactions and excitons 194
11.2 Distributed transition moments 197
11.3 Interactions involving open-shell systems 199
12 Practical Models for Intermolecular Potentials 201
12.1 Potentials for atoms 202
12.2 Model potentials for molecules 209
12.3 Dependence on internal coordinates 219
12.4 A case study: potentials for water 225
12.5 Coarse-grained models 229
12.6 Calculation of energy derivatives 229
12.7 Derivatives with respect to orientation 231
 Contents xi

13 Theory and Experiment 240

13.1 Properties of individual molecules 240
13.2 Validation of intermolecular potentials by experimental methods 244
13.3 Simulation methods 247
13.4 Spectroscopic methods 249
13.5 Molecular beam scattering 260
13.6 Measurements on liquids and solids 263
Appendix A Cartesian Tensors 267
A.1 Basic definitions 267
Appendix B Spherical Tensors 271
B.1 Spherical harmonics 271
B.2 Rotations of the coordinate system 273
B.3 Spherical tensors 274
B.4 Coupling of wavefunctions and spherical tensors 275
Appendix C Introduction to Perturbation Theory 277
C.1 Non-degenerate perturbation theory 277
C.2 The resolvent 280
C.3 Degenerate perturbation theory 280
C.4 Time-dependent perturbation theory 281
Appendix D Conversion Factors 283
D.1 Multipole moments 283
D.2 Polarizabilities 284
D.3 Dispersion coefficients 284
Appendix E Cartesian–Spherical Conversion Tables 285
Appendix F Interaction Functions 291
References 298
Author Index 324
Index 331
This page intentionally left blank
1
Introduction

1.1 The evidence for intermolecular forces

The idea that matter is made up of atoms and molecules was known to the Greeks, though the
evidence for it did not become persuasive until the eighteenth and nineteenth centuries, when
the ideal gas laws, the kinetic theory of gases, Faraday’s laws of electrolysis, the stoichiometry
of most chemical reactions, and a variety of other indications combined to decide the matter
beyond doubt. In the twentieth century, further techniques such as X-ray diffraction and, more
recently, high-resolution microscopy, have provided more evidence.
Given the idea that matter consists of molecules, however, the notion that there must be
forces between them rests on much simpler evidence. The very existence of condensed phases
of matter is conclusive evidence of attractive forces between molecules, for in the absence of
attractive forces, the molecules in a glass of water would have no reason to stay confined to the
glass. Furthermore, the fact that water has a definite density, and cannot easily be compressed
to a smaller volume, shows that at short range the forces between the molecules become
repulsive.
It follows that the energy of interaction U between two molecules, as a function of the
distance R between them, must take the form shown in Fig. 1.1. That is, it must have an
attractive region at long range, where the force −∂U/∂R is negative, and a steeply repulsive
region at close range to account for the low compressibility of condensed materials. There is
a separation Rm where the energy is a minimum, and a closer distance σ where the energy
of interaction goes through zero before climbing steeply. These are conventional notations,
as is the symbol  for the depth of the attractive well. The precise form of the function U(R)
will depend on the particular molecules concerned, but these general features will be almost

s R
Rm

–e

Fig. 1.1 A typical intermolecular potential energy function.

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