Issue 2, 2012

Probing structural evolution along multidimensional reaction coordinates with femtosecond stimulated Raman spectroscopy

Abstract

Mapping out multidimensional potential energy surfaces has been a goal of physical chemistry for decades in the quest to both predict and control chemical reactivity. Recently a new spectroscopic approach called Femtosecond Stimulated Raman Spectroscopy or FSRS was introduced that can structurally interrogate multiple dimensions of a reactive potential energy surface. FSRS is an ultrafast laser technique which provides complete time-resolved, background-free Raman spectra in a few laser shots. The FSRS technique provides simultaneous ultrafast time (∼50 fs) and spectral (∼8 cm−1) resolution, thus enabling one to follow reactive structural evolutions as they occur. In this perspective we summarize how FSRS has been used to follow structural dynamics and provide mechanistic detail on three classical chemical reactions: a structural isomerization, an electron transfer reaction, and a proton transfer reaction.

Graphical abstract: Probing structural evolution along multidimensional reaction coordinates with femtosecond stimulated Raman spectroscopy

Article information

Article type
Perspective
Submitted
30 Aug 2011
Accepted
27 Oct 2011
First published
28 Nov 2011

Phys. Chem. Chem. Phys., 2012,14, 405-414

Probing structural evolution along multidimensional reaction coordinates with femtosecond stimulated Raman spectroscopy

R. R. Frontiera, C. Fang, J. Dasgupta and R. A. Mathies, Phys. Chem. Chem. Phys., 2012, 14, 405 DOI: 10.1039/C1CP22767J

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