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  Transient Raman Snapshots of the Twisted Intramolecular Charge Transfer State in a Stilbazolium Dye

Karmakar, S., Ambastha, A., Jha, A., Dharmadhikari, A., Dharmadhikari, J., Venkatramani, R., et al. (2020). Transient Raman Snapshots of the Twisted Intramolecular Charge Transfer State in a Stilbazolium Dye. The Journal of Physical Chemistry Letters, 11(12), 4842-4848. doi:10.1021/acs.jpclett.0c01124.

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 Urheber:
Karmakar, S.1, Autor
Ambastha, A.1, Autor
Jha, A.1, 2, Autor           
Dharmadhikari, A.3, Autor
Dharmadhikari, J.4, Autor
Venkatramani, R.1, Autor
Dasgupta, J.1, Autor
Affiliations:
1Department of Chemical Sciences, TataInstitute of Fundamental Research, ou_persistent22              
2Miller Group, Atomically Resolved Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_1938288              
3Department of Nuclear and Atomic Physics, Tata Institute of Fundamental Research, ou_persistent22              
4Raman Research Institute, Bangalor, ou_persistent22              

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 Zusammenfassung: Optically 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.

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Sprache(n): eng - English
 Datum: 2020-04-102020-05-272020-05-272020-06-18
 Publikationsstatus: Erschienen
 Seiten: 7
 Ort, Verlag, Ausgabe: -
 Inhaltsverzeichnis: -
 Art der Begutachtung: Expertenbegutachtung
 Identifikatoren: DOI: 10.1021/acs.jpclett.0c01124
 Art des Abschluß: -

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Projektname : S.K., A.D., R.V., and J. Dasgupta acknowledge support from the Department of Atomic Energy (DAE), Government of India, under Project No. 12-R&D-TFR-5.10-0100. J. Dasgupta thanks the TIFR high-performance computational facility for support in the computations and the National NMR Facility. The authors like to acknowledge Dr. Alpana Mishra for providing the stilbazolium dye molecule to initiate the project.
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Titel: The Journal of Physical Chemistry Letters
  Kurztitel : J. Phys. Chem. Lett.
Genre der Quelle: Zeitschrift
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Ort, Verlag, Ausgabe: Washington, DC : American Chemical Society
Seiten: - Band / Heft: 11 (12) Artikelnummer: - Start- / Endseite: 4842 - 4848 Identifikator: CoNE: https://pure.mpg.de/cone/journals/resource/1948-7185