jz8b00373_si_liveslides.zip (7.62 MB)
Capturing Structural Snapshots during Photochemical Reactions with Ultrafast Raman Spectroscopy: From Materials Transformation to Biosensor Responses
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posted on 2018-06-22, 16:33 authored by Chong Fang, Longteng Tang, Breland G. Oscar, Cheng ChenChemistry studies the composition,
structure, properties, and transformation
of matter. A mechanistic understanding of the pertinent processes
is required to translate fundamental knowledge into practical applications.
The current development of ultrafast Raman as a powerful time-resolved
vibrational technique, particularly femtosecond stimulated Raman spectroscopy
(FSRS), has shed light on the structure–energy–function
relationships of various photosensitive systems. This Perspective
reviews recent work incorporating optical innovations, including the
broad-band up-converted multicolor array (BUMA) into a tunable FSRS
setup, and demonstrates its resolving power to watch metal speciation
and photolysis, leading to high-quality thin films, and fluorescence
modulation of chimeric protein biosensors for calcium ion imaging.
We discuss advantages of performing FSRS in the mixed time–frequency
domain and present strategies to delineate mechanisms by tracking
low-frequency modes and systematically modifying chemical structures
with specific functional groups. These unique insights at the chemical-bond
level have started to enable the rational design and precise control
of functional molecular machines in optical, materials, energy, and
life sciences.
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Perspective reviewsmetal speciationfluorescence modulationultrafast RamanUltrafast Raman Spectroscopytunable FSRS setupMaterials TransformationRaman spectroscopycalcium ion imagingBiosensor Responses Chemistry studiesbroad-band up-convertedchimeric protein biosensorschemical structuresPhotochemical Reactionstime-resolved vibrational techniqueBUMAlife scienceschemical-bond levelCapturing Structural Snapshots
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