Abstract
Structural dynamics of condensed-phase systems such as fluorescent proteins and biosensors
govern their functions which broadly impact the chemical, biological, and health fields. However, a
complete understanding of their working mechanisms is hindered by the lack of suitable tools that
can resolve atomic motions on intrinsic molecular timescales. This talk presents the table-top
wavelength-tunable femtosecond stimulated Raman spectroscopy (FSRS), aided by transient
absorption spectroscopy and quantum calculations\/molecular dynamics simulations, which have
captured molecular movies of fluorescence and other nonradiative events like never before.
Representative examples include the green and yellow fluorescent protein (GFP\/YFP) from
jellyfish and sea anemone that can be engineered to emit from blue, green to red and sense calcium
(Ca2+) and chloride ions (Cl\u2013) in a ratiometric manner, revealing the ultrafast interplay between
excited-state events such as proton transfer, cis-trans isomerization, dark state formation, and
conformational trapping (rigidity) or switching (flexibility). Such mechanistic understandings have
propelled us to delineate the multidimensional excited- and ground-state potential energy surface
and rationally design\/engineer biomolecular systems with strategic \u201cmicroscopic\u201d modifications
and improved or novel \u201cmacroscopic\u201d functions.
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