Modern Optical Spectroscopy

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1 Modern Optical Spectroscopy With Exercises and Examples from Biophysics and Biochemistry von William W Parson 1. Auflage Springer-Verlag Berlin Heidelberg 2006 Verlag C.H. Beck im Internet: ISBN Zu Leseprobe schnell und portofrei erhältlich bei beck-shop.de DIE FACHBUCHHANDLUNG

2 1 Introduction Overview The Beer Lambert Law Regions of the Electromagnetic Spectrum Absorption Spectra of Proteins and Nucleic Acids Absorption Spectra of Mixtures The Photoelectric Effect Techniques for Measuring Absorbance Pump Probe and Photon-Echo Experiments Linear and Circular Dichroism Distortions of Absorption Spectra by Light Scattering or Nonuniform Distributions of the Absorbing Molecules Fluorescence IR and Raman Spectroscopy Lasers Nomenclature Basic Concepts of Quantum Mechanics Wavefunctions, Operators, and Expectation Values Wavefunctions Operators and Expectation Values The Time-Dependent and Time-Independent Schrödinger Equations Superposition States Spatial Wavefunctions A Free Particle A Particle in a Box The Harmonic Oscillator Atomic Orbitals Molecular Orbitals Approximate Wavefunctions for Large Systems Spin Wavefunctions and Singlet and Triplet States Transitions Between States: Time-Dependent Perturbation Theory Lifetimes of States and the Uncertainty Principle... 68

3 VIII 3 Light Electromagnetic Fields Electrostatic Forces and Fields Electrostatic Potentials Electromagnetic Radiation Energy Density and Irradiance The Complex Electric Susceptibility and Refractive Index Local-Field Correction Factors The Black-Body Radiation Law Linear and Circular Polarization Quantum Theory of Electromagnetic Radiation Superposition States and Interference Effects in Quantum Optics Distribution of Frequencies in Short Pulses of Light Electronic Absorption Interactions of Electrons with Oscillating Electric Fields The Rates of Absorption and Stimulated Emission Transition Dipoles and Dipole Strengths Calculating Transition Dipoles for π Molecular Orbitals Molecular Symmetry and Forbidden and Allowed Transitions Linear Dichroism Configuration Interactions Calculating Electric Transition Dipoles with the Gradient Operator Transition Dipoles for Excitations to Singlet and Triplet States The Born Oppenheimer Approximation, Franck Condon Factors, and the Shapes of Electronic Absorption Bands Spectroscopic Hole-Burning Effects of the Surroundings on Molecular Transition Energies The Electronic Stark Effect Fluorescence The Einstein Coefficients The Stokes Shift The Mirror-Image Law The Strickler Berg Equation and Other Relationships Between Absorption and Fluorescence Quantum Theory of Absorption and Emission Fluorescence Yields and Lifetimes Fluorescent Probes and Tags Photobleaching Fluorescence Anisotropy Single-Molecule Fluorescence and High-Resolution Fluorescence Microscopy Fluorescence Correlation Spectroscopy Intersystem Crossing, Phosphorescence, and Delayed Fluorescence 238

4 IX 6 Vibrational Absorption Vibrational Normal Modes and Wavefunctions Vibrational Excitation IR Spectroscopy of Proteins Vibrational Stark Effects Resonance Energy Transfer Introduction The Förster Theory Exchange Coupling Energy Transfer to and from Carotenoids in Photosynthesis Exciton Interactions Stationary States of Systems with Interacting Molecules Effects of Exciton Interactions on the Absorption Spectra of Oligomers Transition-Monopole Treatments of Interaction Matrix Elements and Mixing with Charge-Transfer Transitions Exciton Absorption Band Shapes and Dynamic Localization of Excitations Exciton States in Photosynthetic Antenna Complexes Excimers and Exciplexes Circular Dichroism Magnetic Transition Dipoles and n π Transitions The Origin of Circular Dichroism Circular Dichroism of Dimers and Higher Oligomers Circular Dichroism of Proteins and Nucleic Acids Magnetic Circular Dichroism Coherence and Dephasing Oscillations Between Quantum States of an Isolated System The Density Matrix The Stochastic Liouville Equation Effects of Stochastic Relaxations on the Dynamics of Quantum Transitions A Density-Matrix Treatment of Steady-State Absorption The Relaxation Matrix More General Relaxation Functions and Spectral Lineshapes Anomalous Fluorescence Anisotropy Pump Probe Spectroscopy, Photon Echoes, and Vibrational Wavepackets First-Order Optical Polarization

5 X 11.2 Third-Order Optical Polarization and Nonlinear Response Functions Pump Probe Spectroscopy Photon Echoes Transient Gratings Vibrational Wavepackets Wavepacket Pictures of Spectroscopic Transitions Raman Scattering and Other Multiphoton Processes Types of Light Scattering The Kramers Heisenberg Dirac Theory The Wavepacket Picture of Resonance Raman Scattering Selection Rules for Raman Scattering Surface-Enhanced Raman Scattering Biophysical Applications of Raman Spectroscopy Coherent Raman Scattering Multiphoton Absorption Quasielastic (Dynamic) Light Scattering (Photon Correlation Spectroscopy) Appendix 1 Vectors 447 Appendix 2 Matrices 451 Appendix 3 Fourier Transforms 455 Appendix 4 Fluorescence Phase Shift and Modulation 459 Appendix 5 CGS and SI Units and Abbreviations 463 References 465 Subject Index 505

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