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

Renee R. Frontiera, Chong Fang, Jyotishman Dasgupta, Richard A. Mathies

Research output: Contribution to journalReview articlepeer-review

55 Scopus citations

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.

Original languageEnglish (US)
Pages (from-to)405-414
Number of pages10
JournalPhysical Chemistry Chemical Physics
Volume14
Issue number2
DOIs
StatePublished - Jan 14 2012

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