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  Torsionally broken symmetry assists infrared excitation of biomimetic charge-coupled nuclear motions in the electronic ground state

Chatterjee, G., Jha, A., Blanco-Gonzalez, A., Tiwari, V., Manathunga, M., Duan, H.-G., et al. (2022). Torsionally broken symmetry assists infrared excitation of biomimetic charge-coupled nuclear motions in the electronic ground state. Chemical Science, 13(32), 9392-9400. doi:10.1039/D2SC02133A.

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 Creators:
Chatterjee, G.1, Author           
Jha, A.1, Author           
Blanco-Gonzalez, A.2, Author
Tiwari, V.1, 3, Author           
Manathunga, M.2, Author
Duan, H.-G.1, Author           
Tellkamp, F.4, Author           
Prokhorenko, V.1, Author           
Ferré, N.5, Author
Dasgupta, J.6, Author
Olivucci, M.2, 7, Author
Miller, R. J. D.8, Author
Affiliations:
1Miller Group, Atomically Resolved Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_1938288              
2Department of Chemistry, Bowling Green State University, ou_persistent22              
3Department of Chemistry, University of Hamburg, ou_persistent22              
4Machine Physics, Scientific Service Units, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_2074322              
5Aix-Marseille Univ, CNRS, ICR, ou_persistent22              
6Department of Chemical Sciences, Tata Institute of Fundamental Research, ou_persistent22              
7Dipartimento di Biotechnologie, Chimica e Farmacia, Università di Siena, ou_persistent22              
8Departments of Chemistry and Physics, University of Toronto, ou_persistent22              

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 Abstract: The concerted interplay between reactive nuclear and electronic motions in molecules actuates chemistry. Here, we demonstrate that out-of-plane torsional deformation and vibrational excitation of stretching motions in the electronic ground state modulate the charge-density distribution in a donor-bridge-acceptor molecule in solution. The vibrationally-induced change, visualised by transient absorption spectroscopy with a mid-infrared pump and a visible probe, is mechanistically resolved by ab initio molecular dynamics simulations. Mapping the potential energy landscape attributes the observed charge-coupled coherent nuclear motions to the population of the initial segment of a double-bond isomerization channel, also seen in biological molecules. Our results illustrate the pivotal role of pre-twisted molecular geometries in enhancing the transfer of vibrational energy to specific molecular modes, prior to thermal redistribution. This motivates the search for synthetic strategies towards achieving potentially new infrared-mediated chemistry.

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Language(s): eng - English
 Dates: 2022-04-132022-07-192022-07-192022-08-28
 Publication Status: Published in print
 Pages: 9
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 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1039/D2SC02133A
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Title: Chemical Science
  Other : Chem. Sci.
Source Genre: Journal
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Publ. Info: Cambridge, UK : Royal Society of Chemistry
Pages: - Volume / Issue: 13 (32) Sequence Number: - Start / End Page: 9392 - 9400 Identifier: ISSN: 2041-6520
CoNE: https://pure.mpg.de/cone/journals/resource/2041-6520