Lecture Notes

Students are encouraged to print and read the course lecture notes in advance of lectures.

A listing of lecture session topics and corresponding lecture notes is included in the table below. In addition, an overall table of contents for the lecture notes is presented.


Lec # Topics
1 Time-Independent Hamiltonian; Two-Level System; Density Matrix (PDF)
2 Time-Development of State Amplitudes: Resonant Driving of a Two-Level System (PDF)
3 Quantum Dynamics; The Time-Evolution Operator (PDF)
4 The Schrödinger, Heisenberg, and Interaction Pictures (PDF)
5 Perturbation Theory I (PDF)
6 Perturbation Theory II
7 Fermi's Golden Rule (PDF)
8 Irreversible Relaxation (PDF)
9 Interaction of Light and Matter; Electric Dipole Hamiltonian (PDF)
10 Electric Dipole Hamiltonian and Absorption of Light (PDF)
11 Spectroscopy of Aggregates (PDF)
12 Spectroscopy of Aggregates (cont.)
13 Time-Correlation Functions (PDF 1) (PDF 2)
14 Absorption Lineshape from Time-Correlation Functions (PDF)
15 Electronic Spectroscopy: The Displaced Harmonic Oscillator Model (PDF)
16 Displaced Harmonic Oscillator
17 Displaced Harmonic Oscillator (cont.)
18 Lineshapes: Fluctuation and Relaxation (PDF)
19 Quantum Fluctuations (PDF)
20 Vibrational Relaxation (PDF)
21 Förster Theory and Marcus Theory (PDF)
22 Linear Response Theory (PDF 1 of 2) (PDF 2 of 2)
23 Nonlinear Spectroscopy I (PDF)
24 Nonlinear Spectroscopy II (PDF)
25 Nonlinear Spectroscopy III (PDF)
26 Nonlinear Spectroscopy IV


Lecture Notes Table of Contents


Topics Lecture Notes Page #
Introduction
Time-Independent Hamiltonian 1
Two-Level System 4
Density Matrix 9
Appendix: Properties of Operators 13
Basics of Time-Dependent Hamiltonian
Resonant Driving of a Two-Level System 14
Quantum Dynamics: The Time-Evolution Operator 20
Schrödinger, Heisenberg and Interaction Pictures 29
Perturbation Theory
First Order Perturbation Theory
37
43
Fermi's Golden Rule 52
Irreversible Relaxation 60
Light-Matter Interaction
Interaction of Light and Matter
Electric Dipole Hamiltonian and Absorption Spectrum
Relaxation and Line Broadening of Spectrum
66
72
74
Supplement: Review of Free Electromagnetic Field 76
Absorption and Stimulated Emission
Spontaneous Emission
81
84
Quantized Radiation Field 86
Absorption Spectra of Molecular Aggregates 97
Spectroscopy Using Time-Correlation Functions
Time-Correlation Functions 110
Supplement: Space Correlation Functions
Absorption Lineshape from Time-Correlation Functions
Examples: Vibrational, Rotational, Raman Spectroscopy
125
129
Ensemble Averaging and Line Broadening 131
Electronic Spectroscopy
The Displaced Harmonic Oscillator Model
Franck-Condon Transitions
Finite Temperature and Coupling to a Distribution
133
139
142
Förster Theory and Marcus Theory 146
Fluctuations and Relaxation Rates
Fluctuations and Spectral Diffusion
Gaussian-Stochastic Model for Lineshape
Appendix: Cumulant Expansion
152
154
160
Quantum Treatment of Fluctuations
Energy Gap Hamiltonian
Brownian Oscillator Model
162
164
173
Vibrational Relaxation 175
Linear Response Theory
Classical Treatment
Linear Response Functions and Susceptibility
Kramers-Krönig Relations
Nonlinear Response Functions
181
186
188
Quantum Response Functions 189
Response Function and Energy Absorption
Relaxation of Prepared State and Fluctuation-Dissipation
193
196
Coherent Nonlinear Spectroscopy
Nonlinear Polarization
Propagating the Density Matrix
198
207
Diagrammatic Perturbation Theory 209
Third-Order Nonlinear Spectroscopy Photon Echo
Transient Grating
CARS
Pump-Probe
212
217
218
220
221
Characterizing Fluctuations with Nonlinear Spectroscopy 223


Acknowledgements

The notes for this course have been developed from many materials. In large part this includes the references for the course, as noted in the readings. I would like to thank a number of colleagues and prior instructors who provided notes that guided the preparation of many of these lectures, including Bob Silbey, Keith Nelson, Bob Field, John Ross and Graham Fleming. I also want to thank Anne Hudson for her invaluable assistance in preparing the notes.