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Multidimensional Vibrational Coherence Spectroscopy

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Abstract

Multidimensional vibrational coherence spectroscopy has been part of laser spectroscopy since the 1990s and its role in several areas of science has continuously been increasing. In this contribution, after introducing the principals of vibrational coherence spectroscopy (VCS), we review the three most widespread experimental methods for multidimensional VCS (multi-VCS), namely femtosecond stimulated Raman spectroscopy, pump-impulsive vibrational spectroscopy, and pump-degenerate four wave-mixing. Focus is given to the generation and typical analysis of the respective signals in the time and spectral domains. Critical aspects of all multidimensional techniques are the challenges in the data interpretation due to the existence of several possible contributions to the observed signals or to optical interferences and how to overcome the corresponding difficulties by exploiting experimental parameters including higher-order nonlinear effects. We overview how multidimensional vibrational coherence spectroscopy can assist a chemist in understanding how molecular structural changes and eventually photochemical reactions take place. In order to illustrate the application of the techniques described in this chapter, two molecular systems are discussed in more detail in regard to the vibrational dynamics in the electronic excited states: (1) carotenoids as a non-reactive system and (2) stilbene derivatives as a reactive system.

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Fig. 1
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Reprinted with permission from Ref. [54]. Copyright 2017 American Chemical Society

Fig. 6

Reprinted from Ref. [57] with the permission of AIP Publishing LLC

Fig. 7

Adapted from Ref. [170]

Fig. 8

Figure adapted with permission from Ref. [69]. Copyright 2013 American Chemical Society

Fig. 9

Reproduced from Ref. [34] with permission from AIP Publishing

Fig. 10

Reprinted from Ref. [20] with the permission of AIP Publishing

Fig. 11

Reprinted from Ref. [77] with permission of ACS https://pubs.acs.org/doi/abs/10.1021%2Fjp5075863

Fig. 12

Reprinted with permission from Ref. [102]. Copyright 2011 American Chemical Society

Fig. 13

Reprinted with permission from Ref. [51]. Copyright 2018 American Chemical Society

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Reprinted with permission from Ref. [77]. Copyright 2014 American Chemical Society https://pubs.acs.org/doi/abs/10.1021%2Fjp5075863

Fig. 16

Adapted with permission from Ref. [54]. Copyright (2017) American Chemical Society

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Authors and Affiliations

  1. Physikalisch-Chemisches Institut, Universität Heidelberg, Im Neuenheimer Feld 229, 69120, Heidelberg, Germany

    Tiago Buckup

  2. Université de Strasbourg, CNRS, Institut de Physique et Chimie des Matériaux de Strasbourg, UMR 7504, and Labex NIE, 67034, Strasbourg, France

    Jérémie Léonard

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Correspondence to Tiago Buckup.

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This article is part of the Topical Collection “Multidimensional Time-Resolved Spectroscopy”; edited by Tiago Buckup and Jeremie Leonard.

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Buckup, T., Léonard, J. Multidimensional Vibrational Coherence Spectroscopy. Top Curr Chem (Z) 376, 35 (2018). https://doi.org/10.1007/s41061-018-0213-4

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