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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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Item Permalink: http://hdl.handle.net/21.11116/0000-0006-C6BC-7 Version Permalink: http://hdl.handle.net/21.11116/0000-0006-C6BD-6
Genre: Journal Article

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https://dx.doi.org/10.1021/acs.jpclett.0c01124 (Publisher version)
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 Creators:
Karmakar, S.1, Author
Ambastha, A.1, Author
Jha, A.1, 2, Author              
Dharmadhikari, A.3, Author
Dharmadhikari, J.4, Author
Venkatramani, R.1, Author
Dasgupta, J.1, Author
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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 Abstract: 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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Language(s): eng - English
 Dates: 2020-04-102020-05-272020-05-272020-06-18
 Publication Status: Published in print
 Pages: 7
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 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1021/acs.jpclett.0c01124
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Title: The Journal of Physical Chemistry Letters
  Abbreviation : J. Phys. Chem. Lett.
Source Genre: Journal
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Publ. Info: Washington, DC : American Chemical Society
Pages: - Volume / Issue: 11 (12) Sequence Number: - Start / End Page: 4842 - 4848 Identifier: CoNE: https://pure.mpg.de/cone/journals/resource/1948-7185