Topics in Current Chemistry

, 375:87 | Cite as

Two-Dimensional Resonance Raman Signatures of Vibronic Coherence Transfer in Chemical Reactions

  • Zhenkun Guo
  • Brian P. Molesky
  • Thomas P. Cheshire
  • Andrew M. Moran
Part of the following topical collections:
  1. Multidimensional Time-Resolved Spectroscopy


Two-dimensional resonance Raman (2DRR) spectroscopy has been developed for studies of photochemical reaction mechanisms and structural heterogeneity in condensed phase systems. 2DRR spectroscopy is motivated by knowledge of non-equilibrium effects that cannot be detected with traditional resonance Raman spectroscopy. For example, 2DRR spectra may reveal correlated distributions of reactant and product geometries in systems that undergo chemical reactions on the femtosecond time scale. Structural heterogeneity in an ensemble may also be reflected in the 2D spectroscopic line shapes of both reactive and non-reactive systems. In this chapter, these capabilities of 2DRR spectroscopy are discussed in the context of recent applications to the photodissociation reactions of triiodide. We show that signatures of “vibronic coherence transfer” in the photodissociation process can be targeted with particular 2DRR pulse sequences. Key differences between the signal generation mechanisms for 2DRR and off-resonant 2D Raman spectroscopy techniques are also addressed. Overall, recent experimental developments and applications of the 2DRR method suggest that it will be a valuable tool for elucidating ultrafast chemical reaction mechanisms.


Multidimensional spectroscopy Raman spectroscopy Ultrafast spectroscopy  Photodissociation Coherence transfer 



This work is supported by the National Science Foundation under CHE-0952439 and CHE-1504350.


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Copyright information

© Springer International Publishing AG 2017

Authors and Affiliations

  • Zhenkun Guo
    • 1
  • Brian P. Molesky
    • 1
  • Thomas P. Cheshire
    • 1
  • Andrew M. Moran
    • 1
  1. 1.Department of ChemistryUniversity of North Carolina at Chapel HillChapel HillUSA

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