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DYNAMICS OF
MOLECULAR EXCITONS
DYNAMICS OF
MOLECULAR EXCITONS

SEOGJOO J. JANG
Queens College, City University of New York
Department of Chemistry and Biochemistry
Queens, NY, United States
Elsevier
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The Boulevard, Langford Lane, Kidlington, Oxford OX5 1GB, United Kingdom
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Copyright © 2020 Elsevier Ltd. All rights reserved.
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noted herein).
Notices
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changes in research methods, professional practices, or medical treatment may become necessary.
Practitioners and researchers must always rely on their own experience and knowledge in evaluating and using any information,
methods, compounds, or experiments described herein. In using such information or methods they should be mindful of their
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Publisher: Matthew Deans

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To my wife
 Contents vii

Contents
About the author . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . xi
Preface . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . xiii
Acknowledgments . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . xv
Chapter 1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1
1.1 Motivation and objective. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1
1.2 Frenkel and Wannier excitons . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3
1.3 Disorder, fluctuations, and measure of delocalization. . . . . . . . . . . . 16
1.4 Utility and limitations of exciton models . . . . . . . . . . . . . . . . . . . . . . . 18
Chapter 2 Microscopic derivation of Frenkel exciton-bath Hamiltonian. 21
2.1 Aggregates of chromophores. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 23
2.2 Aggregates of chromophores embedded in host media . . . . . . . . . 45
2.3 Summary and additional remarks. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 50
Chapter 3 Linear spectroscopy of molecular excitons . . . . . . . . . . . . . . . . 53
3.1 Absorption lineshape . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 57
3.2 Stimulated emission lineshape . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 72
3.3 Model calculations . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 76
3.4 Summary and additional remarks. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 79
Chapter 4 Exciton transfer rates and hopping dynamics . . . . . . . . . . . . . . . 83
4.1 Transfer between two exciton states: Förster theory’s and its
generalizations . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 84
4.2 Transfer between groups of exciton states. . . . . . . . . . . . . . . . . . . . . . 93
4.3 Master equation approaches and long range exciton hopping
dynamics . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 101
4.4 Summary and additional remarks. . . . . . . . . . . . . . . . . . . . . . . . . . . . . 105
Chapter 5 Quantum dynamics of molecular excitons. . . . . . . . . . . . . . . . . 107
5.1 Projection operator formalism . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 109
5.2 Second order approximations . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 118
5.3 Fourth order approximations . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 124
viii Contents

5.4 Harmonic oscillator bath with linear coupling. . . . . . . . . . . . . . . . . . 132

5.5 Summary and additional remarks. . . . . . . . . . . . . . . . . . . . . . . . . . . . . 145

Chapter 6 Excitons and quantum light. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 149

6.1 Interaction of materials with quantum light . . . . . . . . . . . . . . . . . . . . 150
6.2 Microscopic derivation of Förster’s spectral overlap expression . 152
6.3 Polariton. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 157
6.4 Summary and additional remarks. . . . . . . . . . . . . . . . . . . . . . . . . . . . . 159

Chapter 7 Time-resolved nonlinear spectroscopy of excitons. . . . . . . . . 161

7.1 General assumption of material Hamiltonian . . . . . . . . . . . . . . . . . . 162
7.2 Two-pulse spectroscopy . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 164
7.3 Four wave mixing spectroscopy . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 171
7.4 Summary and additional remarks. . . . . . . . . . . . . . . . . . . . . . . . . . . . . 178

Chapter 8 Examples and applications . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 181

8.1 Excitons in natural light harvesting complexes. . . . . . . . . . . . . . . . . 182
8.2 Excitons for photovoltaic devices . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 186
8.3 Excitons for structural determination. . . . . . . . . . . . . . . . . . . . . . . . . . 188
8.4 Summary and additional remarks. . . . . . . . . . . . . . . . . . . . . . . . . . . . . 192

Chapter 9 Summary and outlook. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 195

Appendix A Useful mathematical identities and solutions. . . . . . . . . . . . 199
A.1 Solution of eigenvalue problems for the simple Frenkel exciton
models . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 199
A.2 Some identities for averages involving harmonic oscillator
models . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 201
Appendix B Interaction between matter and classical
electromagnetic fields . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 207
B.1 Maxwell equations . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 207
B.2 Classical Hamiltonian for matter and radiation interaction . . . . . . 213
B.3 Quantum mechanical Hamiltonian for matter-radiation
interaction in the weak field limit with Coulomb gauge . . . . . . . . . 214
 Contents ix

B.4 Interaction with a plane wave radiation and dipole

approximation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 215

Bibliography . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 219
Index . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 223
 About the author xi

About the author

Seogjoo J. Jang is a Professor of Chemistry at Queens College of
the City University of New York (CUNY), and is a doctoral fac-
ulty of both Chemistry and Physics PhD programs at the Graduate
Center of CUNY. He obtained his BS (1989) and MS (1993) degrees
in Chemistry from Seoul National University, and a PhD degree
(1999) in Chemistry from the University of Pennsylvania. He then
worked as a postdoctoral associate at MIT (1999–2002) and as a
Goldhaber Distinguished Fellow (2003–2005) at Brookhaven Na-
tional Laboratory before starting his faculty position at Queens
College, CUNY in 2005. His research expertise is in quantum dy-
namics theories and computational modeling. In particular, he
has pioneered modern theories of resonance energy transfer that
are now being incorporated into theoretical analyses of experi-
mental data on complex molecular systems, and has made key
contributions to understanding the role of delocalized excitons
in photosynthetic light harvesting complexes. He is a recipient of
the National Science Foundation CAREER Award (2009) and the
Camille Dreyfus Teacher Scholar Award (2010).
 Preface xiii

Preface

Writing a book on exciton is an act of significant courage given

that there are already many authoritative classic books on this
topic that are hard to match. However, when Prof. David Andrews
invited me to write a book on molecular excitons as one of the
Nanophotonics Series, I accepted the offer without much hesi-
tation. I hoped writing such a book would be a great chance to
organize the information and knowledge I have cumulated over
about two decades of research. In addition, throughout my inter-
actions with colleagues and students, I have indeed experienced
the necessity for a new kind of monograph on excitons that can
address current computational and experimental need, in partic-
ular concerning the dynamics.
This book is intended for general readers who have completed
standard graduate level quantum mechanics or quantum chem-
istry courses. I tried to make this book as a kind of self contained
theoretical reference for those who try to understand theories of
exciton dynamics. This book can help non-experts who would
like to get into this field of research and also experts by offering
new details and perspectives that are not often discussed explic-
itly. I tried to also address applications as much as possible, but I
should admit that the account of applications in this book is quite
limited.
There are three major issues this book is particularly focused
on. The first is to understand the assumptions and approxima-
tions implicit in conventional models for molecular excitons and
their interactions with environments. Most of consideration is at
formal level, which will form the basis for more detailed numerical
investigations in the future. In addition, this part can be consid-
ered as an extension of standard molecular quantum mechanics,
and can be used as supplemental reading for a quantum chem-
istry class. The second is to offer as comprehensive description
as possible of most dynamics theories of molecular excitons. The
main focus was on explaining the derivation of these theories and
methods. The rate theories and quantum dynamics methods de-
scribed here are in fact much more general and are applicable to
other quantum dynamical processes. Finally, detailed theoretical
description is provided for the spectroscopy of excitons. Again, the
major focus is on theoretical aspects of these spectroscopic meth-
xiv Preface

ods and understanding their capability as a tool for probing the

exciton dynamics.

Seogjoo J. Jang
New York
December 6, 2019
 Acknowledgments xv

Acknowledgments

I thank the late Bob Silbey who taught me a great deal about
molecular excitons when I was a postdoctoral researcher at MIT.
He also continued inspiring me for many years afterwards as a
colleague. Interactions with him were always special. He could
easily explain important ideas and issues in a few minutes, which
helped me understand their implications so quickly and pursue
new ideas efficiently. Writing this book gave me another chance
to interact with him indirectly through his publications, and I am
still learning from works he has completed decades ago.
Although not directly related to this topic, I am heavily in-
debted to Marshall Newton, one of the best critical thinker and
theoretician I am aware of. His broad knowledge and expertise in
electron transfer theories helped me envision a roadmap for de-
veloping theories of exciton transfer and dynamics, which have
remained relatively unexplored in comparison to the field of elec-
tron transfer theories. Communications and interactions with him
helped me evolve through my early formative period as an inde-
pendent theoretician.
There are also many others that I should not forget mention-
ing names for various contributions related to this book. I am
indebted to my mentors at Seoul National University, Sangyoub
Lee and Kook Joe Shin, who first introduced me to Förster theory
and guided my first research on this topic, and to my PhD mentor
Gregory Voth from whom I learned the fundamentals of quantum
dynamics. I would like to thank Jeff Cina, David Reichman, Chris
Bardeen, Yuan-Chung Cheng, Benedetta Mennucci, Joe Subotnik,
Dorthe Eisele, Greg Scholes, Young Min Rhee, David Coker, Jian-
shu Cao, Jasper Knoester, Graham Fleming, and K. Birgitta Whaley
for discussions and help at various stages leading to this work,
and Frank Spano, Ari Chakraborty, Qiang Shi, and Andrew Mar-
cus for allowing me use their images. Support from National Sci-
ence Foundation, the Department of Energy, and Camille Dreyfus
Foundation have made it possible to continue projects that con-
stitute various parts of this book.
I am grateful to the editor of the Nanophotonics Series, Prof.
David Andrews, and the editorial office of Elsevier for support. Fi-
nally, I cannot thank enough my wife who has been truly support-
ive of writing this book. I am happy to dedicate this book to her.

Seogjoo J. Jang
January 28, 2020
Introduction
1
Contents
1.1 Motivation and objective 1
1.2 Frenkel and Wannier excitons 3
1.2.1 A brief overview 3
1.2.2 Model Hamiltonians for Frenkel excitons 6
1.2.2.1 Linear chain 7
1.2.2.2 Circular chain 11
1.2.3 Semiclassical model Hamiltonians for Wannier excitons 15
1.3 Disorder, fluctuations, and measure of delocalization 16
1.4 Utility and limitations of exciton models 18

1.1 Motivation and objective

An exciton represents a quantum mechanical state of elec-
tronic excitation or a bound pair of an electron and its hole.1
Any electronic excitation of a molecule can be viewed as an ex-
citon confined within the molecule. However, the real benefit of
the concept of exciton is that it helps generalizing the excitation
beyond molecular boundaries in a simple manner. For example,
excitons can be formed across the confines of molecules and exist
in quantum mechanical superposition states. These represent col-
lective quantum states distinctive from independent sums of ele-
mentary molecular excitations, which can exhibit unique quan-
tum mechanical properties of collective nature. One well-known
example is the super-radiance, a collective emission phenomenon
that applies to any atomic [1] or molecular systems [2–6].
Direct experimental confirmation of molecular excitons was
difficult in early days of quantum mechanics. Although well-
established conceptually, their practical significance was not
clearly recognized either. Through decades of research and devel-
opment, excitons have steadily become established as essential
objects for solar light harvesting, imaging, sensing, lasing, and
light-emitting devices. Applications of excitons for quantum infor-
mation processing devices and novel photonic materials are also
emerging areas of research. Thanks to these advances, excitons
are now well supported by many computational and experimental
1 The hole itself is a quasi-particle and refers to the absence of electron.

Dynamics of Molecular Excitons. https://doi.org/10.1016/B978-0-08-102335-8.00009-0 1

Copyright © 2020 Elsevier Ltd. All rights reserved.
2 Chapter 1 Introduction

data, and are perceived as important objects for a few key applica-
tions. However, while data informing the existence and contribu-
tion of excitons abound, accurate and complete information on
excitons is still difficult to get in general. In particular, accurate
measurement of both spatial patterns and temporal dynamics of
excitons, which is crucial for satisfactory microscopic characteri-
zation, remains a challenging area of research even to date.
The difficulty in detailed microscopic characterization of ex-
citons stems in part from their indefinite spatial extents (in
nanometer length scales) and transient dynamical nature (in time
scales typically as short as tens of femtoseconds). Resolving this
issue requires experimental tools that can simultaneously probe
nanometer length scales at femtosecond time resolution, which
remain challenging despite recent advances. The other reason, al-
though less appreciated, is the fact that exciton has often been
perceived by experimentalists as a loosely defined simple object of
semi-empirical nature. This is in contrast to the current status of
computational molecular quantum mechanics, which has come a
long way of constructing sophisticated methods and rigorous mi-
croscopic formulations that can account for various many-body
quantum effects. The gap between these modern practices of
molecular quantum mechanics and the conceptual basis of most
experimental investigation based on old exciton theories, is often
the source of confusion and miscommunication.
For both practical and fundamental reasons, there is increas-
ing demand for accurate characterization and control of excitons
in complex environments. However, for many interesting systems,
the scale and accuracy of calculations necessary for reliable com-
putation of excitonic properties is in general beyond the reach of
rigorous computational methods at present. Significant theoreti-
cal progress is needed for more accurate and microscopic descrip-
tion of excitons as well as for further advances in experimental
probe techniques. In promoting the theoretical progress, it is im-
portant to establish a general theoretical framework for excitons
that is both rigorous and practical. This is one of the main motiva-
tions for this book.
The first objective of this book is to help consolidating many
versions and ideas of excitons into a single theoretical formalism.
While this is an ambitious objective difficult to achieve at present,
this book can set the stage for initiating a long term effort of such
nature. In addition, many assumptions and approximations clar-
ified in this book will help gain better understanding of the dy-
namics and spectroscopic data. The second objective is to offer
comprehensive description of various theories of exciton dynam-
ics along with their applications. There are multiple approaches
 Chapter 1 Introduction 3

possible for achieving this goal. The approach taken in this book
is to begin with molecular Hamiltonians. This approach makes
it straightforward to clarify assumptions and approximations im-
plicit in different forms of excitons from the outset. The formal
foundation for this will be provided in the next chapter. In the
rest of this chapter, for motivational purposes, a brief overview of
Frenkel and Wannier excitons is presented. This is then followed
by introduction of simple model Hamiltonians used for describ-
ing such excitons.
A few words on the convention of notations. For exciton states
and Hamiltonians, the first order quantization and the Dirac no-
tation for states and operators will be used in most cases. The sec-
ond quantization will be primarily reserved only for the descrip-
tion of electromagnetic radiation within the quantum electrody-
namics formalism. When appropriate, semiclassical description
of electromagnetic radiation will also be used for the description
of matter-radiation interaction.

1.2 Frenkel and Wannier excitons

1.2.1 A brief overview
Frenkel [7–9] and Wannier excitons [10,8] represent two well-
known forms of collective excitations that are applicable in two
opposing limits and are amenable for simple quantum mechani-
cal description.
Frenkel exciton theory has been successful for describing the
spectroscopy of molecular crystals and aggregates [8,11,12], where
molecules are bound together by weak interactions. In this case,
electronic properties of individual molecules remain mostly in-
tact. Thus, collective excitation processes can be described still
in terms of properties characterizing the excitation of individual
molecules. Application of the Frenkel exciton theory has since
been expanded to macromolecular and supramolecular systems.
Most recently, Frenkel excitons were shown to play a major role in
natural photosynthetic light harvesting complexes [13].
On the other hand, Wannier excitons [10,8] are appropriate for
inorganic insulating or semiconducting solid materials where the
band theory serves as a successful framework to describe delocal-
ized electrons and holes. The concept of Wannier exciton played
a key role in the development of inorganic photovoltaic and solid
state laser devices. To a certain extent, Wannier excitons can be
used to describe electronic excitation processes in highly confined
systems such as quantum dots.
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