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LECTURES ON LIGHT
Lectures on Light
Nonlinear and Quantum Optics using the Density Matrix
Second Edition
Stephen C. Rand
University of Michigan, USA
3
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
© Stephen C. Rand 2016
The moral rights of the author have been asserted
First Edition published in 2010
Second Edition published in 2016
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
Published in the United States of America by Oxford University Press
198 Madison Avenue, New York, NY 10016, United States of America
British Library Cataloguing in Publication Data
Data available
Library of Congress Control Number: 2016930235
ISBN 978–0–19–875745–0
Printed and bound by
CPI Group (UK) Ltd, Croydon, CR0 4YY
Preface to the First Edition
This book, and the course from which it sprang, attempts to bridge the enormous gap
between introductory quantum mechanics and the research front of modern optics and
other fields that make use of light. This would be an impossibly daunting task, were
it not for the fact that most of us love to hear things again and again that we already
know. Taking that into account, this book uses a single approach repeatedly to tackle
progressively more exciting topics in the science of light, moving systematically and
swiftly from very basic concepts to sophisticated topics.
The reader should be aware from the outset that the approach taken here is uncon-
ventional. It is highly selective instead of encyclopedic, and it teaches the reader only
how to use the density matrix on new problems. Nowadays scientific answers are being
sought to an ever-expanding array of problems across numerous disciplines. The trend
in textbooks on quantum optics is understandably to cover an increasing number of top-
ics comprehensively, and to familiarize students with an ever-widening array of analytic
tools, exhaustively. There are many fine texts that fulfill this function, but this book is
not one of them. Instead, important topics and alternative methods of analysis have been
omitted here to keep it as brief as possible, with a single-minded pedagogical purpose
in mind. The main objective of the book is to provide students and researchers with
one reliable tool, and the confidence that comes from practice, to analyze new optical
phenomena in their chosen field successfully and rigorously.
Thus, the one and only analytic tool developed here for attacking research-level
problems in optical science is the density matrix. A systematic procedure is applied to
representative problems of “critical subjects”—usually only one example each—to show
how virtually any problem can be analyzed with the density matrix. Each successive
example adds one system property at a time, with the result that one qualitatively new
feature appears in the dynamics each time. By using a systematic “building-up” prin-
ciple to approach complicated interactions, students begin to recognize what terms in
the analysis are associated with particular changes in the dynamics. Following two slow-
paced introductory chapters on review material, the text shifts focus to the development
of insights as to when atomic motion, or multi-level structure, or coherence effects dom-
inate the behavior of complicated systems. It ends with fast-paced coverage of selected
topics and applications.
The organization of the book follows the original sequence of lectures on light pre-
pared for applied physics graduates with typical undergraduate physics, chemistry and
engineering preparation, expected to handle interdisciplinary research topics during
their careers. Present day graduate students who use light often face important prob-
lems that no longer fall into the neat categories of unique models from the early days of
quantum mechanics, and require broad perspective and reliable mathematical tools to
vi Preface to the First Edition
handle new cross-disciplinary topics quickly. This course therefore embraces not only
students from traditional subject areas that make use of light (physics, chemistry, elec-
trical engineering, materials science), but also the biophysicist who needs laser tweezers,
the photochemist who wants coherent control, the biomedical engineer who needs to
image through scattering media, the mechanical engineer interested in molecular design
of new materials, and others. The greatest theoretical challenge faced by most students
is to make appropriate connections between standard models and the bewildering land-
scape of new research questions on intersecting boundaries of “hyphenated” subjects
like biophysics, biomedicine, photochemistry, etc. For them, the systematic progression
of Lectures on Light offers an approach to quantum optical analysis that should help
bridge the gaps.
Why choose the density matrix? After all, there are many mathematical tools available
to treat nonlinear and quantum optics. The answer is that the density matrix has features
that make it a natural choice. For example it permits one to ignore parts of a problem
that appear to be irrelevant and to focus mathematically on the dynamics of interest to
the researcher. Also, if desired, it can be reduced to a rate equation treatment—a familiar
approach to analysis that all students of science encounter. In addition, it is particularly
well suited for dealing with coherence in isolated or interactive systems.
This makes it an excellent point of departure for anyone who wishes to use light either
to probe or control systems about which little is known. By focusing on this adaptable
tool, readers can cover a lot of intellectual ground with the minimum investment in
mathematical complexity. What emerges is a reliable analytic framework for use in any
research where light probes or controls or alters a system, regardless of whether the
problems are classical or quantum.
Another hurdle that is addressed explicitly in this book, and that is very important,
is the persistent issue of whether simplified models provide reliable representations of
complicated systems. That is why the last part of Chapter 3 examines in detail the ques-
tion of whether sodium atoms can ever legitimately be viewed as two-level systems given
the complexity of their energy level structure. It turns out the experimentalist is much
more in control of the effective number of levels than one might guess. By the end of
this course, graduate students in interdisciplinary science are able to exercise consider-
able judgment in the creation of useful models for their own frontier research problems
and analyze them by drawing on solid examples and the explicit methodology of the text.
Some familiarity with introductory quantum mechanics is assumed. However, ad-
vanced preparation in optics is not essential to learn and use this material. Over the years,
students from disciplines as diverse as the ones mentioned above—mechanical engi-
neering, materials science, electrical, and biomedical engineering together with physics,
applied physics, and chemistry—have found it to provide the essential insights and
analysis they need for immediate application in their research. Some material that is or-
dinarily omitted from advanced quantum mechanics texts is included to set the stage for
the broadest possible applicability. An example of this is third order perturbation theory.
This topic provides an important bridge to understanding nonlinear behavior of even
the simplest quantum mechanical systems. Since self-saturation effects, cross-saturation,
four-wave mixing processes, and other third order phenomena are encountered much
Preface to the First Edition vii
more commonly in pump–probe experiments than one might expect, it is important that
readers become familiar with third order effects early in the course of their research. An-
other unusual feature of this book is that a few procedural errors are presented early on
to illustrate what can go wrong when quantum mechanical calculations are formulated
inconsistently. These humbling examples remind us all that in research, and most espe-
cially in cross-disciplinary work, there is no substitute for the use of common sense and
no shortcut to pioneering science.
This book progresses as rapidly as possible from a simple and easy review to challeng-
ing modern applications. One layer of conceptual or computational complexity is added
in each new section. The technical material begins with some uncommon examples of
introductory quantum mechanics that force students from the start to revisit the basic
physical principles of optics and quantum mechanics studied as undergraduates. Poten-
tial pitfalls are also pointed out that arise from the inclusion of relaxation processes in
system dynamics. Once the density matrix approach to dynamics is motivated, formu-
lated and understood, the course progresses at an accelerated rate through important
applications. Hence the material is best studied in sequence.
This lecture material will be most useful to students interested in acquiring rigorous,
broadly-applicable analysis quickly. However, the systematic application of one mathe-
matical tool to many forefront topics in nonlinear and quantum optics will be of interest
to seasoned researchers as well. The heavy reliance in late chapters on the insights
and dynamic effects described in earlier chapters helps to keep the treatment short.
Much of the course relies on the semi-classical description in which only the atoms are
quantized—the light field is not. This is intended to encourage intuitive thinking to as
late a stage as possible. However, in the last two chapters several topics are covered where
both the atoms and the light field are quantized and intuitive notions are sometimes poor
guides. Finally, the selected research topics of Chapter 7 not only illustrate the power of
systematic density matrix analysis but give students confidence that, as they approach
the exciting frontiers of their own research, the combination of density matrix analysis
and common sense perspectives developed throughout this course will facilitate success.
I would like to acknowledge all the help I have received during various stages of prep-
aration of this monograph. First and foremost, I am grateful for the comments and
questions of students who took this course over a period of two decades. Along with
my own graduate students, they helped to make the presentation compact by forcing
me to provide concise answers about confusing notions. I am indebted to Philbrick
Bridgess of Roxbury Latin School for imparting to me his respect for analytic geom-
etry, which ultimately led to the discovery of transverse optical magnetism, covered in
Section 7.4 of this book. On a few topics I have drawn liberally from existing texts,
but most especially from Elements of Quantum Optics by Meystre and Sargent, Quantum
Electronics by Yariv, Quantum Optics by Zhubary and Scully, Laser Physics by Sargent,
Scully, and Lamb, Optical Resonance and Two-Level Atoms by Allen and Eberly, and
Foundations of Laser Spectroscopy by Stenholm. I am thankful for their fine examples
of concise pedagogy. Also I thank my colleagues at the University of Michigan for cre-
ating the intellectual environment that made this book possible. Support was provided
by the Department of Electrical Engineering and Computer Science for typing of a
viii Preface to the First Edition
rough draft by Ruby Sowards, Nick Taylor, and Susan Charnley. The graduate student
course itself was offered through the Department of Physics. I owe a debt of gratitude
to Kevin Rand for preparing many original illustrations and for the adaptation of pub-
lished figures. The cover diagram was furnished by William Fisher. I am particularly
grateful to Boris Stoicheff, Richard Brewer, Art Schawlow, Ted Hansch, and Juan Lam
for their friendship and for sharing what they knew. Their examples were inspirational.
Finally, I am deeply indebted to my family—especially my wife Paula who patiently
endured the taxing process of finalizing the manuscript.
S.C. Rand
February 27, 2010
Preface to the Second Edition
In the years following the first edition of this book, some topics have been added in
response to student interest in research advances. These have now been incorporated
in the new edition, making it more comprehensive in its coverage of advanced research.
However by continuing to emphasize compact descriptions it has been possible to keep
the book close to its original length even though the number of problems at the ends
of chapters has doubled. Many students and colleagues have provided suggestions and
corrections to improve the presentation and I gratefully acknowledge their input. I would
especially like to thank Hope Wilson, Alex Fisher, Hamed Razavi, and Austin Tai for
help preparing new figures in Chapters 5, 6, and 7.
S.C. Rand
October 29, 2015
Contents
Appendices
Appendix A Expectation Values 331
Appendix B The Heisenberg Uncertainty Principle 332
Appendix C The Classical Hamiltonian of Electromagnetic Interactions 335
Appendix D Stationary and Time-Dependent Perturbation Theory 338
Appendix E Second Quantization of Fermions 345
Appendix F Frequency Shifts and Decay Due to Reservoir Coupling 349
Appendix G Solving for Off-Diagonal Density Matrix Elements 353
Appendix H Irreducible Spherical Tensor Operators and the
Wigner–Eckart Theorem 356
Appendix I Derivation of Effective Hamiltonians 368
Appendix J Irreducible Representation of Magnetic Dipole Interactions 370
Index 373
1
Basic Classical Concepts
1.1 Introduction
In classical physics, light interacts with matter as described by a compact set of equations
formulated by James Clerk Maxwell in 1865, namely Maxwell’s equations. Solutions for
the propagation of electromagnetic fields in arbitrary media can generally be built up
from solutions to these equations for individual frequency components, and are particu-
larly easy to find if the fields have slowly varying electric and magnetic field magnitudes.
The medium through which light passes must also be uniform and the timescale of inter-
est must greatly exceed the optical period. Fortunately, these conditions are not terribly
restrictive. They encompass most (though not all) distinctive phenomena in classical as
well as quantum optics. Perhaps more importantly, they form a useful framework for
lectures on light without unnecessarily limiting our horizons.
Nowadays, the optical characteristics of media can often be engineered to enhance
specific interactions deliberately. For example, quasi-phase-matching crystals can be
prepared with periodically inverted domain structure to allow the build-up of new fre-
quency components in the optical field. Similarly, in so-called metamaterials, deliberate
variation in microstructure from point to point within a medium is intended to permit
light fields to evolve in complicated but controllable ways. It has been shown in recent
years that metamaterials can be designed to distort the way electromagnetic waves move
through an occupied region of space, in such a way as to render objects located there
effectively invisible. Yet even the passage of light through these non-uniform media is
again entirely predictable using Maxwell’s equations and modern computational tools.
The relative maturity of the subject of electromagnetism and the power of modern com-
puters have put us in a position to predict in great detail how light moves, and how it is
attenuated, emitted, amplified, or scattered as it progresses through practically any kind
of matter. So why is it that light is still such a vital topic today, and when do we have to
treat problems quantum mechanically? How can it be that so many new marvels have
emerged from the study of electromagnetism and optical science in the last decade or
two? The pace of major discoveries continues unabated. How can light tantalize and sur-
prise experts in the twenty-first century with an ever-expanding landscape of discovery
and applications at a time when Maxwell’s equations are 150 years old?
In addition to being a manual for applications of the density matrix, this book seeks
to answer this question. One of its goals is to teach students how to explore and analyze
the unknown without already knowing everything. For this journey, the density matrix
is a perfect companion, since one finds that with it the wavefunction of complex sys-
tems is no longer needed to calculate most things of interest in optical interactions. The
content of this course has been presented now for two decades as an advanced lecture
course on light for graduate students at the University of Michigan—primarily those
with backgrounds in physics, chemistry, and engineering. It seeks to give students fa-
miliarity with a single analytic tool, the density matrix, by applying it systematically to
a great many forefront problems in modern optics. It presents a concise, broad (though
admittedly incomplete) picture of active research fronts in optical science that students
can absorb in a single semester. It does not pretend to be a comprehensive reference
for research in any specialty area from which one or more examples may have been
drawn. Instead, it shows students how to get started on virtually any research problem
using a standard toolbox, and gives them the requisite perspective on what is physically
possible and essential in the analysis. Students acquire a sense for when classical, semi-
classical, or quantum optical approaches need to be applied, when coherence plays an
important role and when it does not, when an exact solution is required and when it is
not, through an approach that adds one concept at a time systematically with a single
mathematical tool.
Among the more advanced topics that are included in this course are free induction
decay, photon echoes, nutation, spectral and spatial hole-burning, light shifts, two- and
three-level coherence, Zeeman coherence, coherent population transfer, electromagnet-
ically induced transparency, slow light, high-order perturbation theory, laser cooling,
optical magnetism, squeezed light, dressed atoms, quantum computation, and cavity
quantum electrodynamics. Although some of these subjects are typically omitted from
standard textbooks on light, experience has shown they can be handled by intermediate
or beginning graduate students when the progression through these topics is presented
in sufficiently small steps. Moreover, this process succeeds in providing a framework
for understanding optical phenomena in a way that is quite different from that of books
that emphasize a sequence of different mathematical techniques to handle quantum me-
chanics. For this reason, most of the book utilizes a “semi-classical” approach that treats
the system under study as a quantum system but avoids the introduction of operators to
describe the electromagnetic field itself. This has the merit of postponing operator math-
ematics required for the quantization of the electromagnetic field until the final chapters
when they are really needed.
Analysis of many forefront topics in optics with a single approach gives readers con-
fidence that they can proceed into virtually any developing field where light is used to
probe or control dynamics, and confidently formulate an initial attack on their research
problem. Naturally it also has the disadvantage of being just one approach. Many of us
are familiar with the mathematical handicap that can result from a bad choice of co-
ordinate system, or an ill-suited choice of variables. However, the density matrix is a
remarkably complete and forgiving tool that accomplishes the essential things. First, it
incorporates the all-important phases of fields and polarizations responsible for some
Electric and Magnetic Interactions 3
∂ D̄
∇¯ × H̄ = J¯ + , (1.2.1)
∂t
∂ B̄
∇¯ × Ē = – , (1.2.2)
∂t
∇¯ · D̄ = ρv , (1.2.3)
∇¯ · B̄ = 0. (1.2.4)
4 Basic Classical Concepts
(1)
and the relative, linear dielectric constant εr = ε/ε0 is given by εr = 1 + χe .
In nonlinear or strongly excited media, there are higher order terms that intro-
(1) (2)
duce field-induced effects. That is, P = P (1) + P (2) + . . . = ε0 (χe E + χe E 2 + . . .).
We deal with nonlinear response when multi-photon transitions of isolated atoms are
considered in later chapters. Nonlinear response can also arise from the finite response
time of bound electrons or charge motion in the case of free carriers. Either mech-
anism can produce a “nonlocal” relationship between the polarization and the field.
That is, P(r̄, t) ≈ ε0 χe (t – t , r̄ – r̄ )E(r̄ , t ). If we are interested only in slow dynamics in
dielectrics we can often ignore such effects. However, finite response times cannot be
ignored on ultrafast timescales in semiconductors, plasmas, or organic electronic mater-
ials. They also cannot be ignored in photorefractive media, where charges diffuse slowly
from place to place, or in multi-level media where long-lived states lead to time-delayed
response.
∂ J¯ ∂ 2E ∂ 2 P̄ ∂ M̄
= –μ0 – μ0 ε0 2 – μ0 2 – μ0 ∇¯ × . (1.2.8)
∂t ∂t ∂t ∂t
Electric and Magnetic Interactions 5
∇¯
∇¯ × ∇¯ × Ē = –∇ 2 Ē + ∇¯ ∇¯ · Ē = –∇ 2 E + ∇¯ · D̄ – ∇¯ · P̄ . (1.2.9)
ε
Provided that the local free charge density ρv is zero and there are no spatial variations
of polarization due to charge migration or field gradients, we find ∇¯ · D̄ = ∇¯ · P̄ = 0 and
in free space the wave equation becomes
1 ∂ 2 Ē ∂ 2 P̄
∇ 2 Ē – = μ 0 , (1.2.10)
c2 ∂t2 ∂t2
1
Ē(z, t) = E0x (z)x̂ exp[i(kz – ωt)] + c.c., (1.2.11)
2
where c.c. stands for complex conjugate. Other possible polarization states are con-
sidered in Section 1.2.6. Here however we show, by substituting Eq. (1.2.11) into
Eq. (1.2.10), that the wave equation can often be written in a scalar form that ignores
the vector character of light. After substitution, the orientation of the field emerges as a
common factor, which may therefore simply be dropped from the equation. In this way,
we find
∂E0x (z) ω2 ω2
2ik – k2 – 2 E0x (z) = – χe E0x (z). (1.2.13)
∂z c c2
6 Basic Classical Concepts
ω2
k2 = 2
1 + χ . (1.2.14)
c
This relationship between frequency ω and wavenumber k is known as the linear
dispersion relation. It is a defining relationship for light, usually written as
ω = cn k, (1.2.15)
where cn (ω) = c/n(ω) is the phase velocity of the wave in which c is the speed of light in
vacuum and n is the refractive index given by n2 = 1 + χ . Equating the imaginary parts
of Eq. (1.2.13), one finds
∂E0x (z) ω2
2k = – 2 χ E0x (z). (1.2.16)
∂z c
∗
Multiplication of both sides of Eq. (1.2.16) by the conjugate field amplitude E0x (z) yields
∂|E0 |2 ω2 χ
=– 2 |E0 |2 , (1.2.17)
∂z c k
and thus
∂I
= –αI , (1.2.18)
∂z
where I is the optical intensity and α is the absorption coefficient, defined by
ω2 χ
α≡ . (1.2.19)
c2 k
In vacuum this result is just α = kχ . The solution of Eq. (1.2.18) can be written as
which is Beer’s law. When α > 0, the electromagnetic wave undergoes exponential ab-
sorption (loss). When α < 0, there is exponential amplification (gain). Beer’s law applies
to optical propagation in many systems. Exceptions include systems where radiation
trapping, saturation, or multiple scattering take place.
such as the dependence of the phase velocity cn on refractive index and the exponential
nature of absorption/gain in simple materials. However, to this point we have no model
or fundamental theory for the electric susceptibility χ itself.
For this purpose we turn to a classical harmonic oscillator model based on linear re-
sponse (and Hooke’s law). The electron and proton comprising a fictitious atom are
joined by a mechanical spring with a restoring force constant k0 . It is assumed the pro-
ton does not move significantly in response to the applied field (Born approximation),
whereas the displacement x(t) about equilibrium of the bound electron depends on the
applied field according to F̄ = –eĒ = –k0 x̄. If Ē is harmonic in time, solutions will have
the form x(t) = x0 exp(–iωt). Upon substitution into Newton’s second law
∂ 2 x(t) ∂x(t)
me – me γ + k0 x(t) = –eE0x exp(–iωt), (1.2.21)
∂t2 ∂t
one can solve for the amplitude x(t) of driven charge motion, which is given by
eE0x /me
x0 = , (1.2.22)
ω2 – iωγ – ω02
√
where ω0 ≡ k0 /me is the resonant frequency of the oscillator and γ is an empirical
damping constant. The total polarization is
N
P(t) = – ex(t) = –Nex(t), (1.2.23)
1
1.8
1.6
1.4
1.2
1.0
n
0.8
0.6
0.4
0.2
0.0
–10 –5 0 5 10
(ω0 – ω)/Γ
Figure 1.1 Frequency dependence of absorption (solid curve) and dispersion (refractive index; dashed
curve) near a resonance at frequency ω0 in the classical model.
In Section 1.2.4, the polarization of light was introduced as a property of light specify-
ing the direction in which the optical electric field is oriented. Since the field orientation
may vary in time, this definition still admits three fundamentally different states of po-
larization which are called linear, right circular, and left circular. Linear polarization
describes light waves in which the electric field points in a fixed direction. For exam-
ple, x-polarized light propagating along ẑ has an E field oriented along the unit vector x̂.
Hence it may be written in the form Ē(z, t) = Ex (z, t)x̂ or Ē(z, t) = E(z, t)eˆ if we let ê rep-
resent a more general polarization unit vector. Circular polarization describes light with
an electric field vector that executes a circle around the propagation axis. The electric
field rotates once per cycle, either clockwise or counterclockwise, as the wave propagates
forward. The circular basis vectors for these polarizations are
√
ε̂± = ∓ 1/ 2 (x̂ ± i ŷ). (1.2.24)
In the case of circular polarization, the vector ê = ε̂ ± is an axial rather than a polar vector.
The 90◦ difference in phase of oscillations along x̂ and ŷ in Eq. (1.2.24) results in fields
of the form Ē(z, t) = Ex (z, t)ε̂± that do not point in a fixed direction. Instead, they
rotate as the wave propagates. Circular and linear states of polarization are illustrated in
Figure 1.2.
Circular polarizations carry spin angular momentum of ±h̄, as indicated in Figure 1.2.
The field direction and the energy density associated with the field twists as it moves,
undergoing a helical rotation with respect to ẑ. Linear polarization carries no angular
momentum, since the electric field vector does not rotate about ẑ at all. This latter state
of polarization is a special combination or superposition state, consisting of the sum of
two equal-amplitude, circularly polarized fields of opposite helicity.
Supplementary Reading 9
–ћ σ–
Lin
ear
σ+
+ћ
Figure 1.2 Fundamental polarizations of light, illustrating light fields that carry spin angular momenta
of –h̄, 0, and +h̄ (top to bottom, respectively). Angular momentum carried by a light wave affects the way
it interacts with matter.
Exercise: (a) Show that light which is linearly polarized along x̂ can be written as the
sum of two opposite circularly polarized fields. That is, show from Eq. (1.2.24)
that x-polarized light is a phased, superposition state of two equal amplitude right
and left circularly polarized components:
√
x̂ = – 1/ 2 (ε̂+ – ε̂ – ). (1.2.25)
Since momentum must be conserved in optical interactions, just as energy must be con-
served, we can anticipate that any angular momentum carried by light may affect the
way it interacts with materials. This point is addressed in later chapters.
..........................................................................................................
S U P P L E M E N TA RY R E A D I N G
where ν0 is called the transition frequency. Individual transitions are rarely observable
because even small particles of bulk matter contain a great many atoms, and light of
even modest intensity I ∝ |E|2 consists of a high density (N/V = I /chν) of energy-bearing
particles (photons) which cause transitions at random times. So individual interactions
generally go unnoticed. Particle-like interactions of light waves are rarely observed un-
less intensities are extremely low. If a light field is pictured as a collection of quantum
particles of energy hν0 , then at low intensity the particles must be widely separated in
time, presuming they are all the same. We then require a description of light in terms
of mathematical operators that produce discrete changes of the field when they interact.
The particle nature of light is therefore an important factor determining the noise and
statistical correlation properties of weak fields. However, a great many important aspects
of light–matter interactions can be described adequately by treating only the atomic vari-
ables quantum mechanically as operators and the light field classically, with an amplitude
and phase that are continuous scalar functions. This approach, called the semi-classical
approach, is the one adopted throughout the first few chapters of this book. Aspects of
light–matter interactions that depend explicitly on the discrete character of the field are
reserved for the final chapters.
Charge motion caused by light is typically a dipolar response such as that determined
in our classical model (Eq. (1.2.21)). However, in systems of bound charges excited near
internal resonant frequencies, the dipole polarization that develops must clearly depend
on the stationary quantum states and the corresponding resonant frequencies. Hence
under these conditions, polarization of the medium becomes a quantum mechanical
observable determined to first order by non-zero values of the first moment of the mi-
croscopic polarization operator p̂. Hence we shall need a procedure for determining the
expected values of the dipole moment and other operators weighted by available states
of the atomic system (specified by the probability amplitude ψ of finding the system in
a given state at a given time and location) to predict the outcome of experimental meas-
urements. This predictor of repeated measurements is called the expectation value, and
it resembles an average weighted by the probability amplitude of the state of the system.
The most important physical observable considered throughout this book is the electric
dipole p̂ = –er̄, which has an expectation value given by
p̂ = – ψ|er¯ |ψ ≡ –e ψ ∗ r̄ψdV . (2.1.3)
Here the wavefunction ψ(r, t) accounts for the proportion of eigenstates contributing to
the actual state of the system. (See Section 2.2 and Appendix A for a more complete dis-
cussion of the definition of expectation value.) The bra-ket symbols used in Eq. (2.1.3)
were introduced by Dirac to represent not only the conjugate state functions ψ ↔ |ψ
and ψ ∗ ↔ ψ| respectively but also to simplify spatial integrals where |ψ and ψ| appear
in combination, as in the dipole moment ψ|er̄ |ψ of Eq. (2.1.3). This notation provides
a convenient shorthand and will be used to shorten calculations throughout the book.
The total polarization for N identical atomic dipoles in the quantum mechanical
limit is obtained by summing individual contributions with an expression similar to
12 Basic Quantum Mechanics
Eq. (1.2.21). However, the notation now implicitly includes functions (wavefunctions)
on which the operator of interest must operate for the expression to have meaning:
N
P̄ = – er̄ i . (2.1.4)
i=1
Dipoles may be static or time varying. When P̄ is time varying, it may have observable
effects even if its time average is zero, because the charge distribution oscillates and may
cause a change of state of the atom or lead to radiation. Indeed, the magnitude of the
dipole operator er̄ evaluated between different states of a single atom, molecule, or optical
center will be shown to be the dominant factor determining the rate of optically induced
transitions between quantum states. For a collection of atoms however, we shall find that
the relative phase variation of er¯i from one atom to the next also plays an important
role in determining the magnitude and temporal development of the ensemble-averaged
or macroscopic polarization P̄ in Eq. (2.1.4). The behavior of P̄ due to initial phas-
ing, dephasing, and even rephasing is important in coherent optical processes, and the
density matrix is especially well-suited to keep track of important phase information.
∆kx = k0∆ θ
k0 ∆x
z
Figure 2.1 Illustration of a typical uncertainty relationship between spatial resolution x and the cor-
responding angular spread that accompanies optical diffraction at an aperture according to the relation
px x = h̄k0 θ x ≥ h̄/2.
The exact form of this Heisenberg uncertainty relation is justified and generalized in
Appendix B for all pairs of conjugate variables. A simple example of the reciprocal re-
lationship between spatial and angular resolution governed by Eq. (2.2.2) is illustrated
by diffraction from an aperture (Figure 2.1), when a plane wave develops a spread of
propagation directions as it passes through a small aperture.
Measurements acquire minimum uncertainty when the product in Eq. (2.2.2) takes
on its minimum value. For the variables in the previous paragraph, the minimum prod-
uct is px x = h̄/2. When systems are prepared in minimum uncertainty or coherent
states they obey this equality, as discussed in Chapter 6. However, it will be shown that
despite the inescapable uncertainty associated with wave mechanics, the Heisenberg limit
expressed by Eq. (2.2.2) can be partly circumvented by preparing systems in special
states called coherent states.
is a particular solution which satisfies Schrödinger’s equation when the system energy is
constant (i.e., Ĥ ψn = i h̄ ∂t∂ ψn = h̄ωn ψn and h̄ωn must be the energy eigenvalue E of the
spatial eigenstate):
Ĥ Un = h̄ωn Un .
The energy of real, non-decaying systems is constant and observable, so the eigenvalues
of such systems are real. It is the adjoint nature of Ĥ that assures us mathematically
that the eigenvalues are real, that the corresponding eigenfunctions Un can be or-
thonormalized, and that they collectively furnish a complete description of the system.
That is,
Un∗ Um d 3 r = δnm , (2.2.6)
Un∗ (r̄)Un (r̄ ) = δ r̄ – r̄ . (2.2.7)
Formally, the Un form a complete basis set that can represent an arbitrary state of the sys-
tem. The most general solution for the wavefunction is formed from linear combinations
of solutions like Eq. (2.2.5), such as
If the total probability |ψ|2 for the system to occupy the space defined by the basis
functions Un is to be normalized to unity, one can easily show from Eq. (2.2.8) that the
constant coefficients must satisfy
|Cn |2 = 1. (2.2.9)
n
Quantum Observables 15
In Eq. (2.2.9), |Cn |2 gives the occupation probability associated with a particular eigen-
state labeled by index n. This closure relation is exploited in Section 2.4 as the main tool
for changing between alternative descriptions of a system, expressed in terms of various
basis sets.
2.2.3 Symmetry
When researchers are confronted by a new problem, the greatest simplifications arise
from considering system symmetries. Symmetry can be exploited to reduce complex
problems to simpler ones and to derive general rules for atom–field interactions. The
optimal approach to using symmetry in this way is the domain of group theory, which
is too extensive a topic to be included here. However, we review one symmetry here,
inversion symmetry, because it has important implications for many problems in optical
science. It affects both linear and nonlinear interactions of light with matter. In a later
chapter we shall encounter the Wigner–Eckart theorem (see also Appendix H) which
can be used to implement other symmetry considerations, without group theory. For a
broader discussion of symmetry, see Ref. [2.2].
When a system has inversion symmetry, it is energetically indistinguishable in inverted
and non-inverted states (see Figure 2.2). Then, one can conclude from symmetry alone
that (i) the wavefunctions for different stationary states may be classified into odd or even
“parity,” (ii) the system cannot sustain a permanent dipole moment, and (iii) “parity”
must change when an electromagnetic transition occurs. Hence the presence or absence
of this symmetry often determines whether electromagnetic transitions are allowed or
not. To confirm these results we introduce parity operator Iˆ, defined by its inverting
action on all three spatial coordinates, and allow it to operate on the energy eigenvalue
equation:
Iˆ Ĥ (r̄)ψ(r̄) = IˆEψ(r̄) = Eψ(–r̄). (2.2.10)
Figure 2.2 Example of a three-dimensional object with inversion symmetry. A featureless sphere looks
the same if the coordinates are all reversed.
16 Basic Quantum Mechanics
since Ĥ (r̄) = Ĥ (–r̄). This last point is the result of the system being physically indistin-
guishable in inverted or non-inverted states. Eq. (2.2.11) shows that the commutator
[Ĥ , Iˆ] = 0. Since Iˆ commutes with Ĥ , the energy eigenfunctions of Ĥ are also eigen-
functions of Iˆ. The eigenvalues I of the parity operator are easily found by applying
inversion twice to return the original wavefunction. Thus
Iˆ2 ψ = I 2 ψ = ψ, (2.2.12)
and wavefunctions of the system separate into two groups distinguished by I = ±1.
In the presence of inversion symmetry we reach three conclusions:
ψ|er|ψ = 0, (2.2.15)
regardless of the state ψ of the system.
3. Transition dipole moments (where the initial and final states are different) only
exist between states of opposite parity.
(o) (e)
ψ (r) er ψ (r) = Iˆ ψ (o) (r) er ψ (e) (r) = –ψ (o) (r) –er ψ (e) (r)
= ψ (o) (r) er ψ (e) (r) = 0, (2.2.16)
(o) (o) (o) (o) (o) (o) (o) (o)
ψ1 er ψ2 = Iˆ ψ1 er ψ2 = –ψ1 –er –ψ2 = – ψ1 er ψ2 = 0,
(2.2.17)
(e) (e) (e) (e) (e) (e) (e) (e)
ψ1 er ψ2 = Iˆ ψ1 er ψ2 = ψ1 –er ψ2 = – ψ1 er ψ2 = 0.
(2.2.18)
These selection rules based on inversion symmetry play an important role in some
of the simple examples of quantum systems that follow.
Quantum Observables 17
mω0 ½
Un = √ n Hn (ξ ) exp(–ξ 2 /2), (2.2.20)
h̄ π 2 n!
√
where ξ ≡ mω0 /h̄x and Hn (ξ ) is a Hermite polynomial. These will later be referred to
as basis states and written simply as |n ≡ |Un . The eigenvalues are
1
h̄ωn = n + h̄ω0 , n = 0, 1, 2, . . . (2.2.21)
2
Note that the eigenfunctions separate into even and odd sets, reflecting the inversion
symmetry of the motion about the origin.
2
Energy (ћω0 )
n=0
–2 –1 ξ=0 1 2
Figure 2.3 The lowest three eigenfunctions of the simple harmonic oscillator.
18 Basic Quantum Mechanics
where kn = nπ /L and n = 1, 2, 3, . . .
The energy eigenvalues are
h̄2 k2n
h̄ωn = , (2.2.24)
2m
and a general wavefunction for this problem is
1/2
2
ψ= Cn sin (kn z) e–iωn t . (2.2.25)
L n
Notice that the solutions in Eq. (2.2.25) again separate into contributions with n even or
odd, reflecting the inversion symmetry of the potential, as in Section 2.2.3.
ћωn
4
3
2
1
z
0 L
Figure 2.4 The two lowest eigenfunctions of a one-dimensional infinite square well.
Quantum Observables 19
Strained
GaN
AlGaN
2DEG
EC
V(x)
E3
E2
E1
Figure 2.5 (a) Schematic cross-section of a ternary nitride semiconductor structure giving rise to a two-
dimensional electron gas (2DEG) at the AlGaN/GaN interface (in the middle). (b) The linear potential
well and quantized energy levels at the 2DEG interface.
1/3
En 2me V0
ξn ≡ x – , (2.2.28)
V0 h̄2
where n = 1, 2, 3, . . . is an integer index for the various solutions, this equation simpli-
fies to
d2
– ξ n Un (ξn ) = 0. (2.2.29)
dξn2
20 Basic Quantum Mechanics
The solution of this equation is an Airy function, related to Bessel functions of fractional
order. A suitable integral form of this function can be written as
∞
1 1 3
n (ξn ) = cos u + uξn du, (2.2.30)
π 3
0
where An is a constant amplitude for the nth solution. To find energy eigenvalues it is
necessary to apply boundary conditions. For this we can approximate the well height at
the origin as infinite, so that U (ξ ) = 0 at x = 0. That is,
1/3
En 2me V0
Un – = Un (–Rn ) = 0. (2.2.32)
V0 h̄2
This shows that the eigenvalues are proportional to roots (Rn ) of the Airy function. The
first few roots are R1 = 2.34, R2 = 4.09, R3 = 5.52, and R4 = 6.78. Hence the eigenvalues,
obtained from Eq. (2.2.32), are
1/3
V02 h̄2
En = Rn . (2.2.33)
2me
∞
Un∗ (ξ )Un (ξ )dξ = |An |2 , (2.2.34)
–Rn
In this example, no reduction of the wavefunction into sets of even and odd energy
levels takes place. Because of the lack of inversion symmetry, the wavefunctions do not
separate into different parity classes. (See Handbook of Mathematical Functions, NBS,
1964, pp.446–447, Eqs. 10.4.1 and 10.4.32 and Ref. [2.3]).
Quantum Observables 21
where kx = πa nx , ky = πa ny , and kz = π
n.
a z
The energy eigenvalues are
h̄2 k2 h̄2 k2x + k2y + k2z h̄2 π 2 2
E n x , ny , nz = = = n + n2y + n2z . (2.2.37)
2m 2m 2ma2 x
The ground state energy is
3h2
E0 = , (2.2.38)
8ma2
since nx = ny = nz = 1. The energy of the first excited state is
6h2
E1 = , (2.2.39)
8ma2
since nx = 2 and ny = nz = 1. The transition frequency of the first resonance of the
F center is therefore given by
3n2
hν = E1 – E0 = , (2.2.40)
8ma2
from which one obtains directly the Mollwo–Ivey relation [2.4] for the relationship
between the edge length of the crystal unit cell and the frequency of resonant absorption:
1
ln(a) = ln(ν) + c. (2.2.41)
2
As shown in Figure 2.7, this relation has been confirmed by measurements on various
alkali halide crystals.
22 Basic Quantum Mechanics
(a) z
2
) y
2 ψ(y
ψ (z)
ψ(x) 2
(b) z
2
) y
2 ψ(y
)
ψ(z
ψ(x) 2
Figure 2.6 Pictorial representation of the wavefunctions and charge distributions of an F center in the
(a) ground state and (b) the first excited state. (After Ref. [2.4]).
Multi-electron color centers are not only good examples of particle-in-a-box anal-
ysis, but have been widely used in high-gain tunable laser technology [2.5]. Another
important application relies on their mobility under applied fields. Oxygen vacancies
in semiconducting rutile (TiO2 ) are thermally more stable than the alkali F centers
and can be made to migrate by the application of voltage across the crystal, causing
a change in resistance of the medium proportional to the integral of voltage over time.
This understanding led to the first realization of a fundamental circuit element called the
memristor [2.6].
Dynamics of Two-Level Systems 23
1.0
KI
KCl
0.6 KBr LiCl
NaCl
a (nm)
LiF
NaF
0.4
0.3
3 5 10 15
vmax(1014 Hz)
Figure 2.7 Plot of experimental measurements of the first absorption resonance of F centers in several
alkali halides, compared with the prediction of the Mollwo–Ivey relation (solid curve). (After Ref. [2.4].)
Since the light field is under the experimentalist’s control, assume it is a plane wave
traveling along z with no variation of its amplitude in x or y. The dipole moment could
be oriented in an arbitrary, fixed direction described by
μ̄ = μx x̂ + μy ŷ + μz ẑ. (2.3.2)
Perpendicular to z, only the x and y components of the moment are relevant for interac-
tion with the wave. In free space the orientation of Ē is perpendicular to the direction of
propagation, so μz ẑ · Ē(z, t) = 0. Since we are told the absorption is isotropic, we may
also assume μx = μy = μ0 , and without loss of generality reduce Eq. (2.3.1) to
where E0 is the amplitude of the electromagnetic wave. The charge oscillations excited
by the field are restricted to the x–y plane. So the interaction spans a two-dimensional
Hilbert space. Equation (2.3.3) therefore describes a 2-D interaction operator, and can
be represented using 2×2 matrices—the Pauli spin matrices which (together with the
unit matrix σI ) form a complete basis set:
0 1 0 –i 1 0
σ̂x = ; σ̂y = ; σ̂z = . (2.3.4)
1 0 i 0 0 –1
This set of matrices is called complete because any complex two-component vector can
be written as a linear combination of σx , σy , and σz together with the unit matrix σI using
appropriate coefficients. Also, the product of any two Pauli matrices is a Pauli matrix,
showing that they form a complete group. Since light can at most transform the state
of the atom among its available states in Hilbert space, the interaction Hamiltonian Ĥ I
must be an operator that can convert a 2-vector into another 2-vector in the same Hilbert
space. So its matrix representation must also be 2×2 and we choose the Pauli matrices
0
as basis operators. The operator representation of Eq. (2.3.3) must change state
1
1
into and vice versa. Hence it is given by
0
Exercise: Confirm that the form of Ĥ I in Eq. (2.3.5) is correct by applying it to ei-
ther eigenstate of the two-level atom and showing that it causes a transition to the
other.
Dynamics of Two-Level Systems 25
Now σ̂x can be written in terms of raising and lowering operators for atomic states to
simplify interpretation of dynamics. Consider the following two matrices.
1 0 1 0 1
σ̂ + ≡ σ̂x + i σ̂y = → σ̂ + = , (2.3.6)
2 0 0 1 0
1 0 0 1 0
σ̂ – ≡ σ̂x – i σ̂y = → σ̂ – = . (2.3.7)
2 1 0 0 1
Writing the interaction Hamiltonian in terms of these operators, which raise or lower the
state of the atom, Eq. (2.3.5) becomes
0 1
Ĥ int = –μ0 E0 = –μ0 E0 σ̂ + + σ̂ – . (2.3.8)
1 0
It may now be deduced that a continuous field–atom interaction causes the atom to
make periodic transitions up and down between states 1 and 2 by stimulated absorption
and emission, respectively, at a frequency related to the absorption coefficient (since it
depends on the transition moment μ0 ).
As shown by the exercise, discrete applications of the interaction Hamiltonian show
the individual transitions caused by optical irradiation:
0 1
Ĥ int = –μ0 E0 (2.3.9)
1 0
and
1 0
Ĥ int = –μ0 E0 . (2.3.10)
0 1
A more detailed picture of system dynamics can only emerge by solving explicitly for
temporal evolution of the state of the system. In the present problem there is no infor-
mation on the stationary states of the system. So we do not know the wavefunction itself,
but we do know there are at least two states in the system. There is a ground state which
might be represented as ψ – and an excited state ψ + . The challenge of predicting what
the system will do in response to irradiation requires the determination of the most gen-
eral wavefunction we can write based on this information. This is ψ(t) = c+ ψ + + c– ψ – ,
where c+ and c– are time-dependent coefficients. So the time-dependent Schrödinger
equation yields
d +
c (t)ψ + + c– (t)ψ – = iΩ σ̂ + + σ̂ – c+ (t)ψ + + c– (t)ψ –
dt
= i c+ (t)ψ – + c– (t)ψ + , (2.3.11)
26 Basic Quantum Mechanics
and because ψ + and ψ – are independent vector states, Eq. (2.3.12) may be decomposed
into the two equations
∂c+
= ic– , (2.3.13)
∂t
∂c–
= ic+ . (2.3.14)
∂t
These two coupled equations are readily solved by differentiation and cross substitution.
∂ 2 c±
= –2 c± (2.3.15)
∂t 2
2
By taking into account the normalization condition c+ + |c– |2 = 1 and initial condition
c– (0) = 1, the overall wavefunction can therefore be written
The system oscillates between the ground state ψ – and the excited state ψ + at a fre-
quency called the resonant Rabi frequency. This oscillatory behavior is called Rabi
flopping. What is interesting here is that we have predicted some system dynamics—an
oscillation at a very specific rate in a poorly characterized system—without knowing the
functional form of the wavefunction ψ or even the unperturbed system Hamiltonian H0 .
It was sufficient to know a little about system symmetry, the energy eigenvalues, and
to assume the optical interaction was dominated by the electric dipole Hamiltonian. It is
particularly important to realize that one can calculate optical properties and dynamic re-
sponse to light without knowing the wavefunction, since the wavefunction itself is rarely
known in systems of interest.
2.4 Representations
2.4.1 Representations of Vector States and Operators
The Hamiltonian describing the interaction of matter with a perturbing influence is often
written as the sum of a static portion Ĥ 0 and an interaction term V̂ (the electric dipole
interaction between light and matter is considered in detail in Appendix C):
Ĥ = Ĥ 0 + V̂ (2.4.1)
Representations 27
d i
|ψ(t) = – Ĥ 0 + V̂ |ψ(t) . (2.4.2)
dt h̄
If the entire Hamiltonian Ĥ itself is time independent, direct integration of Eq. (2.4.2)
yields
i
|ψ(t) = exp – Ĥ t |ψ(0) , (2.4.3)
h̄
showing that the system wavefunction can still evolve by changing the admixture of its
eigenstates. Hence an observable O acquires a time dependence which, if not too rapid,
is reflected in the measured matrix element
Ô(t) = ψ|Ô |ψ . (2.4.4)
There are three common ways to partition the time dependence in Eq. (2.4.4) be-
tween the state vector |ψ and the operator Ô. The most common divisions are the
following:
Schrödinger picture:
S S S
Ô = ψ (t)Ô (0)ψ (t) , (2.4.5)
where ψ S (t) ≡ exp(–i Ĥt/h̄) ψ S (0) .
Interaction picture:
I I I
Ô = ψ (t)Ô (t)ψ (t) , (2.4.6)
where ψ I (t) ≡ exp(i Ĥ 0 t/h̄) ψ S (t) and ÔI (t) ≡ exp(i Ĥ 0 t/h̄)ÔS (0) exp(–i Ĥ0 t/h̄).
Heisenberg picture:
H H H
Ô = ψ Ô (t) ψ , (2.4.7)
where ÔH (t) ≡ exp(i Ĥt/h̄)ÔS (0) exp(–i Ĥt/h̄) and ψ H ≡ ψ S (0) .
These options for representing problems are explored further in the next section. One
of the three pictures is generally preferable to another for a given problem. The choice
of representation is determined by what aspect of system dynamics is to be emphasized
in calculations.
28 Basic Quantum Mechanics
2.4.2.1 Time-Independent Ĥ
Direct integration of the Schrödinger equation when Ĥ is time independent gives
|ψ(t) = exp –i Ĥt/h̄ |ψ(0) , (2.4.8)
where
1 2
exp –i Ĥt/h̄ ≡ 1 – i Ĥt/h̄ – Ĥt/h̄ + . . . (2.4.9)
2
This result can then be used to develop slightly different equations of motion for the
various pictures of system dynamics.
d S
i h̄ ψ (t) = Ĥ ψ S (t) , (2.4.10)
dt
Ô(t) = ψ S (t)Ô(0)ψ S (t) , (2.4.11)
where
S
ψ (t) = exp –i Ĥt/h̄ |ψ(0) . (2.4.12)
In Eq. (2.4.11) the expectation value of the operator has been written in terms
of its initial value Ô(0) to emphasize that it does not change with time. All time
dependence is associated with the wavefunctions in the Schrödinger picture.
Representations 29
Then
d
i h̄ exp –i Ĥ 0 t/h̄ ψ I (t) = Ĥ S0 + V̂ S exp –i Ĥ 0 t/h̄ ψ I (t)
dt
d
i h̄ ψ I (t) = exp i Ĥ 0 t/h̄ V̂ S exp –i Ĥ 0 t/h̄ ψ I (t) .
dt
d I
i h̄ ψ (t) = V̂ I (t) ψ I (t) , (2.4.14)
dt
where
V̂ I (t) ≡ exp i Ĥ 0 t/h̄ V̂ S exp –i Ĥ 0 t/h̄ (2.4.15)
is an effective Hamiltonian for the transformed state vector ψ I (t) . This rep-
resentation is called the interaction
picture, because according to Eq. (2.4.14)
the development of ψ I (t) is determined by the interaction V̂ I (t) alone, rather
than Ĥ 0 or Ĥ .
On the other hand the time development of operators in this picture is deter-
mined by Ĥ 0 . To make a comparison with the Schrödinger picture we note from
Eq. (2.4.15) that an arbitrary operator in the interaction picture relates to one in
the Schrödinger picture according to
ÔI = exp i Ĥ 0 t/h̄ ÔS (0) exp –i Ĥ 0 t/h̄ . (2.4.16)
d I i
Ô (t) = Ĥ 0 , ÔI . (2.4.18)
dt h̄
Note that the expansion coefficients in the Schrödinger and interaction pictures
are different. The complete time dependence is described by Schrödinger coef-
ficients cn (t) in the expansion |ψ = cn (t)|n , whereas the time dependence
n
due only to the interaction is described by interaction picture coefficients Cn (t)
in |ψ = Cn (t) exp(–iωn t)|n . For each eigenfrequency ωn , the coefficients are
n
therefore related by
where
ÔH (t) ≡ exp i Ĥt/h̄ Ô exp –i Ĥt/h̄ (2.4.21)
and
H S
ψ = ψ (0) . (2.4.22)
d H d
ψ = ψ(0) = 0, (2.4.23)
dt dt
d H i H H
Ô = Ĥ , Ô . (2.4.24)
dt h̄
Language: English
BY
FELIX ADLER
Copyright, 1918, by
D. APPLETON AND COMPANY
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