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1 Introduction1

1.1 Overview1

1.2 The Beer-Lambert Law3

1.3 Regions of the Electromagnetic Spectrum4

1.4 Absorption Spectra of Proteins and Nucleic Acids6

1.5 Absorption Spectra of Mixtures8

1.6 The Photoelectric Effect9

1.7 Techniques for Measuring Absorbance10

1.8 Pump-Probe and Photon-Echo Experiments13

1.9 Linear and Circular Dichroism15

1.10 Distortions of Absorption Spectra by Light Scattering or Nonuniform Distributions of the Absorbing Molecules17

1.11 Fluorescence19

1.12 IR and Raman Spectroscopy24

1.13 Lasers25

1.14 Nomenclature26

2 Basic Concepts of Quantum Mechanics29

2.1 Wavefunctions,Operators,and Expectation Values29

2.1.1 Wavefunctions29

2.1.2 Operators and Expectation Values30

2.2 The Time-Dependent and Time-Independent Schr？dinger Equations36

2.2.1 Superposition States41

2.3 Spatial Wavefunctions42

2.3.1 A Free Particle42

2.3.2 A Particle in a Box43

2.3.3 The Harmonic Oscillator46

2.3.4 Atomic Orbitals48

2.3.5 Molecular Orbitals51

2.3.6 Approximate Wavefunctions for Large Systems57

2.4 Spin Wavefunctions and Singlet and Triplet States57

2.5 Transitions Between States：Time-Dependent Perturbation Theory65

2.6 Lifetimes of States and the Uncertainty Principle68

3 Light73

3.1 Electromagnetic Fields73

3.1.1 Electrostatic Forces and Fields73

3.1.2 Electrostatic Potentials74

3.1.3 Electromagnetic Radiation76

3.1.4 Energy Density and Irradiance83

3.1.5 The Complex Electric Susceptibility and Refractive Index90

3.1.6 Local-Field Correction Factors94

3.2 The Black-Body Radiation Law96

3.3 Linear and Circular Polarization98

3.4 Quantum Theory of Electromagnetic Radiation100

3.5 Superposition States and Interference Effects in Quantum Optics104

3.6 Distribution of Frequencies in Short Pulses of Light106

4 Electronic Absorption109

4.1 Interactions of Electrons with Oscillating Electric Fields109

4.2 The Rates of Absorption and Stimulated Emission113

4.3 Transition Dipoles and Dipole Strengths118

4.4 Calculating Transition Dipoles forπMolecular Orbitals126

4.5 Molecular Symmetry and Forbidden and Allowed Transitions128

4.6 Linear Dichroism142

4.7 Configuration Interactions148

4.8 Calculating Electric Transition Dipoles with the Gradient Operator152

4.9 Transition Dipoles for Excitations to Singlet and Triplet States161

4.10 The Born-Oppenheimer Approximation,Franck-Condon Factors,and the Shapes of Electronic Absorption Bands163

4.11 Spectroscopic Hole-Burning171

4.12 Effects of the Surroundings on Molecular Transition Energies174

4.13 The Electronic Stark Effect182

5 Fluorescence189

5.1 The Einstein Coefficients189

5.2 The Stokes Shift192

5.3 The Mirror-Image Law195

5.4 The Strickler-Berg Equation and Other Relationships Between Absorption and Fluorescence197

5.5 Quantum Theory of Absorption and Emission203

5.6 Fluorescence Yields and Lifetimes208

5.7 Fluorescent Probes and Tags214

5.8 Photobleaching218

5.9 Fluorescence Anisotropy219

5.10 Single-Molecule Fluorescence and High-Resolution Fluorescence Microscopy225

5.11 Fluorescence Correlation Spectroscopy231

5.12 Intersystem Crossing,Phosphorescence,and Delayed Fluorescence238

6 Vibrational Absorption241

6.1 Vibrational Normal Modes and Wavefunctions241

6.2 Vibrational Excitation247

6.3 IR Spectroscopy of Proteins253

6.4 Vibrational Stark Effects256

7 Resonance Energy Transfer259

7.1 Introduction259

7.2 The F？rster Theory261

7.3 Exchange Coupling275

7.4 Energy Transfer to and from Carotenoids in Photosynthesis277

8 Exciton Interactions281

8.1 Stationary States of Systems with Interacting Molecules281

8.2 Effects of Exciton Interactions on the Absorption Spectra of Oligomers290

8.3 Transition-Monopole Treatments of Interaction Matrix Elements and Mixing with Charge-Transfer Transitions295

8.4 Exciton Absorption Band Shapes and Dynamic Localization of Excitations298

8.5 Exciton States in Photosynthetic Antenna Complexes301

8.6 Excimers and Exciplexes304

9 Circular Dichroism307

9.1 Magnetic Transition Dipoles and n-π Transitions307

9.2 The Origin of Circular Dichroism317

9.3 Circular Dichroism of Dimers and Higher Oligomers322

9.4 Circular Dichroism of Proteins and Nucleic Acids328

9.5 Magnetic Circular Dichroism332

10 Coherence and Dephasing335

10.1 Oscillations Between Quantum States of an Isolated System335

10.2 The Density Matrix339

10.3 The Stochastic Liouville Equation344

10.4 Effects of Stochastic Relaxations on the Dynamics of Quantum Transitions346

10.5 A Density-Matrix Treatment of Steady-State Absorption352

10.6 The Relaxation Matrix355

10.7 More General Relaxation Functions and Spectral Lineshapes364

10.8 Anomalous Fluorescence Anisotropy370

11 Pump-Probe Spectroscopy,Photon Echoes,and Vibrational Wavepackets377

11.1 First-Order Optical Polarization377

11.2 Third-Order Optical Polarization and Nonlinear Response Functions386

11.3 Pump-Probe Spectroscopy391

11.4 Photon Echoes395

11.5 Transient Gratings401

11.6 Vibrational Wavepackets404

11.7 Wavepacket Pictures of Spectroscopic Transitions413

12 Raman Scattering and Other Multiphoton Processes417

12.1 Types of Light Scattering417

12.2 The Kramers-Heisenberg-Dirac Theory422

12.3 The Wavepacket Picture of Resonance Raman Scattering430

12.4 Selection Rules for Raman Scattering432

12.5 Surface-Enhanced Raman Scattering435

12.6 Biophysical Applications of Raman Spectroscopy436

12.7 Coherent Raman Scattering437

12.8 Multiphoton Absorption439

12.9 Quasielastic(Dynamic)Light Scattering(Photon Correlation Spectroscopy)442

Appendix 1-Vectors447

Appendix 2-Matrices451

Appendix 3-Fourier Transforms455

Appendix 4-Fluorescence Phase Shift and Modulation459

Appendix 5-CGS and SI Units and Abbreviations463

References465

Subject Index505