Two-Dimensional Optical Spectroscopy: 1st Edition (Hardback) book cover

Two-Dimensional Optical Spectroscopy

1st Edition

By Minhaeng Cho

CRC Press

385 pages | 57 B/W Illus.

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Hardback: 9781420084290
pub: 2009-06-16
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Two-Dimensional Optical Spectroscopy discusses the principles and applications of newly emerging two-dimensional vibrational and optical spectroscopy techniques. It provides a detailed account of basic theory required for an understanding of two-dimensional vibrational and electronic spectroscopy. It also bridges the gap between the formal development of nonlinear optical spectroscopy and the application of the theory to explain experimental results.

Focusing on time-domain spectroscopy, the book presents detailed discussions on the underlying physics and interpretation methods of a variety of two-dimensional optical spectroscopic methods. It illustrates how novel diagrammatic techniques are useful in graphically describing the associated nonlinear optical transition pathways and involved population or coherence evolutions. The author also explains the basics of quantum dynamics and time-dependent perturbation theories that are required in describing nonlinear optical processes.

From the development of the theory to novel applications, this book covers a gamut of topics in this field, including perturbation theory, coherent Raman scattering, pump-probe spectroscopy, photon echo spectroscopy, IR-visible four-wave mixing, and linear and nonlinear optical activity spectroscopy. It shows how to apply the recently developed tools of vibrational and electronic spectroscopy in two dimensions.


This is the first book dedicated exclusively to two-dimensional nonlinear optical spectroscopy and is a much needed contribution to the field. … a noteworthy achievement. Cho does an exceptional job of paring down the material into its key components. Along with well-chosen examples, the material is presented in a logical and concise manner. … The book is a valuable resource for experts and nonexperts alike. To the latter, it provides a comprehensive introduction; to the former, it serves as an up-to-date reference source summarizing the current state-of-the-art. In short, it is poised to become the standard text in two-dimensional optical spectroscopy.

—Eric B. Brauns, University of Idaho, writing in Journal of the American Chemical Society

Table of Contents


Quantum Dynamics

Time Evolution in Hilbert Space

Time-Dependent Perturbation Theory in Hilbert Space

Diagram Representation of the Time-Dependent Perturbation Theory in Hilbert Space

Transition Amplitude and Probability in Hilbert Space

Time Evolution in Liouville Space

Time-Dependent Perturbation Theory in Liouville Space

Transition Probability in Liouville Space and Pathways

Linear Response Spectroscopy

Linear Response Function

System-Bath Interaction and Line Broadening

Rotational Averaging of Tensors

Linear Absorption Spectroscopy

Raman Scattering

Hyper-Raman Scattering

IR-Raman Surface Vibrational Spectroscopy

Raman-IR Surface Vibrational Spectroscopy

Appendix: Nonlinear Polarization and Generated Signal Electric Field

Second-Order Response Spectroscopy

Second-Order Response Function

Three-Level System and Line-Broadening Function

Sum-Frequency Generation

Difference-Frequency Generation

IR–IR-vis Four-Wave Mixing

Third-Order Response Spectroscopy

Third-Order Response Function

Four-Level System and Line-Broadening Function

Short-Time Approximation to the Third-Order Response Function

Third-Order Response Function of a Two-Level System

Pump-Probe Spectroscopy of a Two-Level System

Rephasing Photon Echo Spectroscopy of a Two-Level System

Non-Rephasing Photon Echo Spectroscopy of a Two-Level System

Three-Pulse Photon Echo Peak Shift (PEPS)

Two-Dimensional Pump-Probe Spectroscopy

Introduction to Two-Dimensional Pump-Probe Spectroscopy

Two-Dimensional Pump-Probe Spectrum of 2LS

Two-Dimensional Pump-Probe Spectrum of Anharmonic Oscillator

Two-Dimensional Photon Echo Spectroscopy

Phase and Amplitude Detection of Two-Dimensional Photon Echo Signal Field

Two-Dimensional Photon Echo Spectrum: A Two-Level System

Two-Dimensional Non-Rephasing Spectrum: A Two-Level System

Two-Dimensional Photon Echo Spectrum: An Anharmonic Oscillator

Simple Two-Dimensional Lorentzian Peak Shape

Simple Two-Dimensional Gaussian Peak Shape

Coupled Multi-Chromophore System

Frenkel Hamiltonian in Site Representation

Delocalized Exciton Representation

Delocalized State Energy and Transition Dipole Matrix Element

Transition FFCFs

Exchange-Narrowing Effect on Absorption Spectrum

Measurements of Auto and Cross FFCFs

Exciton Population Transfer

Two-Dimensional Spectroscopy of Coupled Dimers

Model Hamiltonian of a Coupled 2LS Dimer

Delocalized Excited-State Energy Fluctuations and Time-Correlation Functions

Coupled 2LS Dimer: Quantum Beats at Short Time

Coupled 2LS Dimer: Intermediate Time Region

Coupled 2LS Dimer: Population Transfer Effects

Coupled Anharmonic Oscillators: Model Hamiltonian

Coupled Anharmonic Oscillators: Two-Dimensional Photon Echo Spectrum at Short Time

Coupled Anharmonic Oscillators: Degenerate Case

Coupled Anharmonic Oscillators: Population Transfer Effects

Chemical Exchange and Two-Dimensional Spectroscopy

Model System

Chemical Exchange Diagrams: Two-Level System

Chemical Exchange Diagrams: Anharmonic Oscillator

Polarization-Controlled Two-Dimensional Spectroscopy

Parallel Polarization ZZZZ-Echo: Two-Level System

Perpendicular Polarization ZYYZ-Echo: Two-Level System

Difference Two-Dimensional Photon Echo Spectrum: Coupled 2LS Dimer

Parallel Polarization ZZZZ-Echo: Anharmonic Oscillators

Perpendicular Polarization ZYYZ-Echo: Anharmonic Oscillators

Difference Two-Dimensional Echo Spectrum: Coupled Anharmonic Oscillators

Generalized Polarization-Controlled Two-Dimensional Spectroscopy

Determination of the Angle between Any Two Transition Dipole Vectors

Applications of Two-Dimensional Vibrational Spectroscopy

Single Anharmonic Oscillator Systems

Coupled Two-Oscillator Systems

Polypeptide Secondary Structures

Globular Proteins and Membrane-Bound Proteins

Nucleic Acids

Hydrogen-Bonding Dynamics and Chemical Exchange

Solute-Solvent Complexation and Micro-Solvation

Internal Rotation

Transient Two-Dimensional IR Spectroscopy: Protein Folding and Unfolding

Applications of Two-Dimensional Electronic Spectroscopy

Application to Fenna-Matthews-Olson Light-Harvesting Complex

Application to Semiconductors

Two-Dimensional Second-Order Response Spectroscopy

Two-Dimensional Sum-Frequency Generation

Two-Dimensional SFG of Solution Sample

Two-Dimensional SFG of Coupled 2LS Dimer

Two-Dimensional SFG of Coupled Anharmonic Oscillators

Two-Dimensional Difference-Frequency Generation

IR–IR-vis SFG and DFG

Other IIV Four-Wave Mixings

Fifth-Order Raman Scattering

Linear Optical Activity Spectroscopy

Radiation-Matter Interaction Hamiltonian and Polarization

Circular Dichroism and Optical Rotatory Dispersion

Raman Optical Activity

IR-Raman Optical Activity Spectroscopy

Raman-IR Optical Activity Spectroscopy

Nonlinear Optical Activity Spectroscopy

Nonlinear Optical Activity Measurement Methods

Rotational Averaging of Higher-Rank Tensors

Two-Dimensional Optical Activity Pump-Probe: Two-Level System

Two-Dimensional Optical Activity Photon Echo: Two-Level System

Two-Dimensional Optical Activity Photon Echo of Coupled 2LS Dimer

References appear at the end of each chapter.

About the Author

Minhaeng Cho is the director of the Center for Multidimensional Spectroscopy at Korea University. A recipient of the Nobel Laureate Signatures Award and Young Scientist Award, Dr. Cho counts theoretical and computational chemistry and experimental ultrafast nonlinear optical spectroscopy among his research interests.

Subject Categories

BISAC Subject Codes/Headings:
MEDICAL / Biochemistry
SCIENCE / Chemistry / Industrial & Technical
SCIENCE / Physics