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Author Valkunas, Leonas
Title Molecular Excitation Dynamics and Relaxation : Quantum Theory and Spectroscopy
Imprint Somerset : John Wiley & Sons, Incorporated, 2013
©2013
book jacket
Edition 1st ed
Descript 1 online resource (465 pages)
text txt rdacontent
computer c rdamedia
online resource cr rdacarrier
Note Molecular Excitation Dynamics and Relaxation -- Contents -- Preface -- Part One Dynamics and Relaxation -- 1 Introduction -- 2 Overview of Classical Physics -- 2.1 Classical Mechanics -- 2.1.1 Concepts of Theoretical Mechanics: Action, Lagrangian, and Lagrange Equations -- 2.1.2 Hamilton Equations -- 2.1.3 Classical Harmonic Oscillator -- 2.2 Classical Electrodynamics -- 2.2.1 Electromagnetic Potentials and the Coulomb Gauge -- 2.2.2 Transverse and Longitudinal Fields -- 2.3 Radiation in Free Space -- 2.3.1 Lagrangian and Hamiltonian of the Free Radiation -- 2.3.2 Modes of the Electromagnetic Field -- 2.4 Light-Matter Interaction -- 2.4.1 Interaction Lagrangian and Correct Canonical Momentum -- 2.4.2 Hamiltonian of the Interacting Particle-Field System -- 2.4.3 Dipole Approximation -- 3 Stochastic Dynamics -- 3.1 Probability and Random Processes -- 3.2 Markov Processes -- 3.3 Master Equation for Stochastic Processes -- 3.3.1 Two-Level System -- 3.4 Fokker-Planck Equation and Diffusion Processes -- 3.5 Deterministic Processes -- 3.6 Diffusive Flow on a Parabolic Potential (a Harmonic Oscillator) -- 3.7 Partially Deterministic Process and the Monte Carlo Simulation of a Stochastic Process -- 3.8 Langevin Equation and Its Relation to the Fokker-Planck Equation -- 4 Quantum Mechanics -- 4.1 Quantum versus Classical -- 4.2 The Schrödinger Equation -- 4.3 Bra-ket Notation -- 4.4 Representations -- 4.4.1 Schrödinger Representation -- 4.4.2 Heisenberg Representation -- 4.4.3 Interaction Representation -- 4.5 Density Matrix -- 4.5.1 Definition -- 4.5.2 Pure versus Mixed States -- 4.5.3 Dynamics in the Liouville Space -- 4.6 Model Systems -- 4.6.1 Harmonic Oscillator -- 4.6.2 Quantum Well -- 4.6.3 Tunneling -- 4.6.4 Two-Level System -- 4.6.5 Periodic Structures and the Kronig-Penney Model -- 4.7 Perturbation Theory
4.7.1 Time-Independent Perturbation Theory -- 4.7.2 Time-Dependent Perturbation Theory -- 4.8 Einstein Coefficients -- 4.9 Second Quantization -- 4.9.1 Bosons and Fermions -- 4.9.2 Photons -- 4.9.3 Coherent States -- 5 Quantum States of Molecules and Aggregates -- 5.1 Potential Energy Surfaces, Adiabatic Approximation -- 5.2 Interaction between Molecules -- 5.3 Excitonically Coupled Dimer -- 5.4 Frenkel Excitons of Molecular Aggregates -- 5.5 Wannier-Mott Excitons -- 5.6 Charge-Transfer Excitons -- 5.7 Vibronic Interaction and Exciton Self-Trapping -- 5.8 Trapped Excitons -- 6 The Concept of Decoherence -- 6.1 Determinism in Quantum Evolution -- 6.2 Entanglement -- 6.3 Creating Entanglement by Interaction -- 6.4 Decoherence -- 6.5 Preferred States -- 6.6 Decoherence in Quantum Random Walk -- 6.7 Quantum Mechanical Measurement -- 6.8 Born Rule -- 6.9 Everett or Relative State Interpretation of Quantum Mechanics -- 6.10 Consequences of Decoherence for Transfer and Relaxation Phenomena -- 7 Statistical Physics -- 7.1 Concepts of Classical Thermodynamics -- 7.2 Microstates, Statistics, and Entropy -- 7.3 Ensembles -- 7.3.1 Microcanonical Ensemble -- 7.3.2 Canonical Ensemble -- 7.3.3 Grand Canonical Ensemble -- 7.4 Canonical Ensemble of Classical Harmonic Oscillators -- 7.5 Quantum Statistics -- 7.6 Canonical Ensemble of Quantum Harmonic Oscillators -- 7.7 Symmetry Properties of Many-Particle Wavefunctions -- 7.7.1 Bose-Einstein Statistics -- 7.7.2 Pauli-Dirac Statistics -- 7.8 Dynamic Properties of an Oscillator at Equilibrium Temperature -- 7.9 Simulation of Stochastic Noise from a Known Correlation Function -- 8 An Oscillator Coupled to a Harmonic Bath -- 8.1 Dissipative Oscillator -- 8.2 Motion of the Classical Oscillator -- 8.3 Quantum Bath -- 8.4 Quantum Harmonic Oscillator and the Bath: Density Matrix Description -- 8.5 Diagonal Fluctuations
8.6 Fluctuations of a Displaced Oscillator -- 9 Projection Operator Approach to Open Quantum Systems -- 9.1 Liouville Formalism -- 9.2 Reduced Density Matrix of Open Systems -- 9.3 Projection (Super)operators -- 9.4 Nakajima-Zwanzig Identity -- 9.5 Convolutionless Identity -- 9.6 Relation between the Projector Equations in Low-Order Perturbation Theory -- 9.7 Projection Operator Technique with State Vectors -- 10 Path Integral Technique in Dissipative Dynamics -- 10.1 General Path Integral -- 10.1.1 Free Particle -- 10.1.2 Classical Brownian Motion -- 10.2 Imaginary-Time Path Integrals -- 10.3 Real-Time Path Integrals and the Feynman-Vernon Action -- 10.4 Quantum Stochastic Process: The Stochastic Schrödinger Equation -- 10.5 Coherent-State Path Integral -- 10.6 Stochastic Liouville Equation -- 11 Perturbative Approach to Exciton Relaxation in Molecular Aggregates -- 11.1 Quantum Master Equation -- 11.2 Second-Order Quantum Master Equation -- 11.3 Relaxation Equations from the Projection Operator Technique -- 11.4 Relaxation of Excitons -- 11.5 Modified Redfield Theory -- 11.6 Förster Energy Transfer Rates -- 11.7 Lindblad Equation Approach to Coherent Exciton Transport -- 11.8 Hierarchical Equations of Motion for Excitons -- 11.9 Weak Interchromophore Coupling Limit -- 11.10 Modeling of Exciton Dynamics in an Excitonic Dimer -- 11.11 Coherent versus Dissipative Dynamics: Relevance for Primary Processes in Photosynthesis -- Part Two Spectroscopy -- 12 Introduction -- 13 Semiclassical Response Theory -- 13.1 Perturbation Expansion of Polarization: Response Functions -- 13.2 First Order Polarization -- 13.2.1 Response Function and Susceptibility -- 13.2.2 Macroscopic Refraction Index and Absorption Coefficient -- 13.3 Nonlinear Polarization and Spectroscopic Signals -- 13.3.1 N-wave Mixing -- 13.3.2 Pump Probe -- 13.3.3 Heterodyne Detection
14 Microscopic Theory of Linear Absorption and Fluorescence -- 14.1 A Model of a Two-State System -- 14.2 Energy Gap Operator -- 14.3 Cumulant Expansion of the First Order Response -- 14.4 Equation of Motion for Optical Coherence -- 14.5 Lifetime Broadening -- 14.6 Inhomogeneous Broadening in Linear Response -- 14.7 Spontaneous Emission -- 14.8 Fluorescence Line-Narrowing -- 14.9 Fluorescence Excitation Spectrum -- 15 Four-Wave Mixing Spectroscopy -- 15.1 Nonlinear Response of Multilevel Systems -- 15.1.1 Two- and Three-Band Molecules -- 15.1.2 Liouville Space Pathways -- 15.1.3 Third Order Polarization in the Rotating Wave Approximation -- 15.1.4 Third Order Polarization in Impulsive Limit -- 15.2 Multilevel System in Contact with the Bath -- 15.2.1 Energy Fluctuations of the General Multilevel System -- 15.2.2 Off-Diagonal Fluctuations and Energy Relaxation -- 15.2.3 Fluctuations in a Coupled Multichromophore System -- 15.2.4 Inter-Band Fluctuations: Relaxation to the Electronic Ground State -- 15.2.5 Energetic Disorder in Four-Wave Mixing -- 15.2.6 Random Orientations of Molecules -- 15.3 Application of the Response Functions to Simple FWM Experiments -- 15.3.1 Photon Echo Peakshift: Learning About System-Bath Interactions -- 15.3.2 Revisiting Pump-Probe -- 15.3.3 Time-Resolved Fluorescence -- 16 Coherent Two-Dimensional Spectroscopy -- 16.1 Two-Dimensional Representation of the Response Functions -- 16.2 Molecular System with Few Excited States -- 16.2.1 Two-State System -- 16.2.2 Damped Vibronic System - Two-Level Molecule -- 16.3 Electronic Dimer -- 16.4 Dimer of Three-Level Chromophores - Vibrational Dimer -- 16.5 Interferences of the 2D Signals: General Discussion Based on an Electronic Dimer -- 16.6 Vibrational vs. Electronic Coherences in 2D Spectrum of Molecular Systems
17 Two Dimensional Spectroscopy Applications for Photosynthetic Excitons -- 17.1 Photosynthetic Molecular Aggregates -- 17.1.1 Fenna-Matthews-Olson Complex -- 17.1.2 LH2 Aggregate of Bacterial Complexes -- 17.1.3 Photosystem I (PS-I) -- 17.1.4 Photosystem II (PS-II) -- 17.2 Simulations of 2D Spectroscopy of Photosynthetic Aggregates -- 17.2.1 Energy Relaxation in FMO Aggregate -- 17.2.2 Energy Relaxation Pathways in PS-I -- 17.2.3 Quantum Transport in PS-II Reaction Center -- 18 Single Molecule Spectroscopy -- 18.1 Historical Overview -- 18.2 How Photosynthetic Proteins Switch -- 18.3 Dichotomous Exciton Model -- Appendix -- A.1 Elements of the Field Theory -- A.2 Characteristic Function and Cumulants -- A.3 Weyl Formula -- A.4 Thermodynamic Potentials and the Partition Function -- A.5 Fourier Transformation -- A.6 Born Rule -- A.7 Green's Function of a Harmonic Oscillator -- A.8 Cumulant Expansion in Quantum Mechanics -- A.8.1 Application to the Double Slit Experiment -- A.8.2 Application to Linear Optical Response -- A.8.3 Application to Third Order Nonlinear Response -- A.9 Matching the Heterodyned FWM Signal with the Pump-Probe -- A.10 Response Functions of an Excitonic System with Diagonal and Off-Diagonal Fluctuations in the Secular Limit -- References -- Index
This work brings together quantum theory and spectroscopy to convey excitation processes to advanced students and specialists wishing to conduct research and understand the entire fi eld rather than just single aspects. Written by experienced authors and recognized authorities in the field, this text covers numerous applications and offers examples taken from different disciplines. As a result, spectroscopists, molecular physicists, physical chemists, and biophysicists will all fi nd this a must-have for their research. Also suitable as supplementary reading in graduate level courses
Description based on publisher supplied metadata and other sources
Electronic reproduction. Ann Arbor, Michigan : ProQuest Ebook Central, 2020. Available via World Wide Web. Access may be limited to ProQuest Ebook Central affiliated libraries
Link Print version: Valkunas, Leonas Molecular Excitation Dynamics and Relaxation : Quantum Theory and Spectroscopy Somerset : John Wiley & Sons, Incorporated,c2013 9783527410088
Subject Condensed matter -- Spectra.;Molecular spectroscopy.;Quantum theory
Electronic books
Alt Author Abramavicius, Darius
Mancal, Tomás
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