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Please use this identifier to cite or link to this item: http://hdl.handle.net/2289/7491
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dc.contributor.authorKarmakar, Shreetama-
dc.contributor.authorAmbastha, Abhinandan-
dc.contributor.authorDharmadhikari, J.A.-
dc.contributor.author+4 Co-Authors-
dc.date.accessioned2020-07-06T08:46:03Z-
dc.date.available2020-07-06T08:46:03Z-
dc.date.issued2020-06-
dc.identifier.citationThe Journal of Physical Chemistry Letters, 2020, Vol.11, p4842−4848en_US
dc.identifier.issn1948-7185-
dc.identifier.urihttp://hdl.handle.net/2289/7491-
dc.descriptionRestricted Accessen_US
dc.description.abstractOptically triggered twisted intramolecular charge transfer (TICT) states in donor–acceptor chromophores form the molecular basis for designing bioimaging probes that sense polarity, microviscosity, and pH in vivo. However, a lack of predictive understanding of the “twist” localization precludes a rational design of TICT-based dyes. Here, using femtosecond stimulated Raman spectroscopy, we reveal a distinct Raman signature of the TICT state for a stilbazolium-class mitochondrial staining dye. Resonance-selective probing of 4-N,N-diethylamino-4″-N′-methyl-stilbazolium tosylate (DEST) tracks the excited-state structure of the dye as it relaxes to a TICT state on a picosecond time scale. The appearance of a remarkably blue-shifted C=C stretching mode at 1650 cm–1 in the TICT state is attributed to the “twist” of a single bond adjacent to the ethylenic π-bridge in the DEST backbone based on detailed electronic structure calculations and vibrational mode analysis. Our work demonstrates that the π-bridge, connecting the donor and acceptor moieties, influences the spatial location of the “twist” and offers a new perspective for designing organelle-specific probes through cogent tuning of backbone dynamics.en_US
dc.language.isoenen_US
dc.publisherAmerican Chemical Societyen_US
dc.relation.urihttps://doi.org/10.1021/acs.jpclett.0c01124en_US
dc.rights2020 American Chemical Societyen_US
dc.titleTransient Raman Snapshots of the Twisted Intramolecular Charge Transfer State in a Stilbazolium Dyeen_US
dc.typeArticleen_US
dc.additionalSupporting Information Availableen_US
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