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.This is the author's peer-reviewed final manuscript, as accepted by the publisher. The published article is copyrighted by the Royal Society of Chemistry and can be found at: http://pubs.rsc.org/en/journals/journalissues/cp
