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Journal ArticleDOI

Four wave mixing spectroscopy for a multilevel system

Jaeyoung Sung, +1 more
- 13 Nov 2001 - 
- Vol. 115, Iss: 20, pp 9266-9287
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TLDR
In this paper, a theory of the four-wave mixing (FWM) spectroscopy for the multilevel system coupled to the bath with arbitrary time scale is presented, in contrast to most previous work that assumes the fast bath dynamic limit.
Abstract
We present a theory of the four-wave-mixing (FWM) spectroscopy for the multilevel system coupled to the bath with arbitrary time scale, in contrast to most previous work that assumes the fast bath dynamic limit (motionally narrowed limit). Exact quantum mechanical expressions for the relevant nonlinear response tensor and the nonlinear polarization vector are obtained for a model Hamiltonian. Effects of molecular rotation and the polarization directions of the input radiation fields are also fully taken into account. The results show how the cross correlation as well as the autocorrelation functions of the fluctuations in the energy-gaps or transition frequencies between eigenstates contribute to the FWM spectroscopy. The result is applied to three-pulse echo spectroscopy. We examine the results for a variety of model spectral density functions, and recover the results of the previously reported theories as limiting cases.

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Two-dimensional femtosecond spectroscopy

TL;DR: This review provides an introduction to two-dimensional Fourier transform experiments exploiting second- and third-order vibrational and electronic nonlinearities.
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Ultrafast hydrogen-bond dynamics in the infrared spectroscopy of water.

TL;DR: Using simulations of an atomistic model of water, this work relates frequency fluctuations in the OH-stretching frequency of HOD in liquid D2O with femtosecond infrared spectroscopy to intermolecular dynamics.
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Coherent Two-Dimensional Optical Spectroscopy

TL;DR: Although the optical analogs of 2D NMR do not provide an atomic resolution structure of complex molecules, optical domain multi-dimensional spectroscopy has certain advantages because of the dramatic gain in time resolution possible and the ability to directly observe and quantify the couplings between quantum states involved in molecular dynamical processes.
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Coherent 2D IR Spectroscopy: Molecular Structure and Dynamics in Solution

TL;DR: In this article, a 2D IR correlation spectrum with absorptive line shapes was obtained from heterodyne-detected third-order nonlinear signals using a sequence of broad bandwidth femtosecond IR pulses.
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Local hydrogen bonding dynamics and collective reorganization in water: ultrafast infrared spectroscopy of HOD/D(2)O.

TL;DR: An investigation into hydrogen bonding dynamics and kinetics in water using femtosecond infrared spectroscopy of the OH stretching vibration of HOD in D(2)O finds a kinetic regime which gives an effective rate for exchange of intermolecular structures.
References
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Book

The Principles of Nonlinear Optics

Y. R. Shen
TL;DR: In this article, the authors present a general description of wave propagation in nonlinear media, including high-resolution nonlinear optical spectroscopy, and four-wave mixing and mixing.
Book

Modern Quantum Mechanics

TL;DR: Modern Quantum Mechanics as mentioned in this paper is a classic graduate level textbook, covering the main quantum mechanics concepts in a clear, organized and engaging manner, and introduces topics that extend the text's usefulness into the twenty-first century, such as advanced mathematical techniques associated with quantum mechanical calculations.
Book

Principles of Nonlinear Optical Spectroscopy

Shaul Mukamel
TL;DR: In this article, the authors present a simulation of the optical response functions of a multilevel system with relaxation in a multimode Brownian Oscillator Model and a wavepacket analysis of nonimpulsive measurements.
Book

Dynamic Light Scattering: With Applications to Chemistry, Biology, and Physics

Bruce J. Berne, +1 more
TL;DR: In this paper, a comprehensive introduction to principles underlying laser light scattering focuses on time dependence of fluctuations in fluid systems and provides an introduction to theory of time correlation functions, with chapters on projection operator techniques in statistical mechanics.
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