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Vibrational energy redistribution during donor–acceptor electronic energy transfer: criteria to identify subsets of active normal modes

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dc.contributor.authorAlfonso Hernández, L.
dc.contributor.authorAthanasopoulos, S.
dc.contributor.authorTretiak, S.
dc.contributor.authorMiguel, B.
dc.contributor.authorBastida, Adolfo
dc.contributor.authorFernández Alberti, S.
dc.contributor.departmentQuímica Física
dc.date.accessioned2024-11-22T12:15:24Z
dc.date.available2024-11-22T12:15:24Z
dc.date.issued2020-07-28
dc.description© the Owner Societies 2020. This document is the Published version of a Published Work that appeared in final form in Physical Chemistry Chemical Physics. To access the final edited and published work see https://doi.org/10.1039/D0CP03102J
dc.description.abstractPhotoinduced electronic energy transfer in conjugated donor–acceptor systems is naturally accompanied by intramolecular vibrational energy redistributions accepting an excess of electronic energy. Herein, we simulate these processes in a covalently linked donor–acceptor molecular dyad system by using nonadiabatic excited state molecular dynamics simulations. We analyze different complementary criteria to systematically identify the subset of vibrational normal modes that actively participate on the donor - acceptor (S2 - S1) electronic relaxation. We analyze energy transfer coordinates in terms of state-specific normal modes defined according to the different potential energy surfaces (PESs) involved. On one hand, we identify those vibrations that contribute the most to the direction of the main driving force on the nuclei during electronic transitions, represented by the non-adiabatic derivative coupling vector between donor and acceptor electronic states. On the other hand, we monitor normal mode transient accumulations of excess energy and their intramolecular energy redistribution fluxes. We observe that the subset of active modes varies according to the PES on which they belong and these modes experience the most significant rearrangements and mixing. Whereas the nuclear motions that promote donor - acceptor energy funneling can be localized mainly on one or two normal modes of the S2 state, they become spread out across multiple normal modes of the S1 state following the energy transfer event.
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dc.format.extent13
dc.identifier.citationPhysical Chemistry Chemical Physics, 2020, Vol. 22, pp. 18454--18466
dc.identifier.doihttps://doi.org/10.1039/D0CP03102J
dc.identifier.issnPrint: 1463-9076
dc.identifier.issnElectronic: 1463-9084
dc.identifier.urihttp://hdl.handle.net/10201/146648
dc.languageenges
dc.publisherRoyal Society of Chemistry
dc.relationThis work was partially supported by CONICET, UNQ, ANPCyT (PICT-2018-2360), the Universidad Carlos III de Madrid, the European Union’s Seventh Framework Programme for research, technological development and demonstration under grant agreement No. 600371, el Ministerio de Economı́a, Industria y Competitividad (COFUND2014-51509), el Ministerio de Educación, cultura y Deporte (CEI-15-17), Banco Santander and el Ministerio de Ciencia, Innovación y Universidades (RTI2018- 101020-B-I00). We also acknowledge support from the Bavarian University Centre for Latin America (BAYLAT). The work at Los Alamos National Laboratory (LANL) was supported by the Laboratory Directed Research and Development Funds (LDRD) program. This work was done in part at the Center for Nonlinear Studies (CNLS) and the Center for Integrated Nanotechnologies (CINT), a U.S. Department of Energy and Office of Basic Energy Sciences user facility, at LANL. This research used resources provided by the LANL Institutional Computing Program. Los Alamos National Laboratory is operated by Triad National Security, LLC, for the National Nuclear Security Administration of the U.S. Department of Energy. This work has received finantial support provided by the Spanish Agencia Estatal de Investigación (AEI) and Fondo Europeo de Desarrollo Regional (FEDER, UE) under Project CTQ2016-79345-P and by the Fundación Séneca under Project 20789/PI/18.es
dc.relation.publisherversionhttps://pubs.rsc.org/en/content/articlelanding/2020/cp/d0cp03102j
dc.rights.accessRightsinfo:eu-repo/semantics/restrictedAccess
dc.titleVibrational energy redistribution during donor–acceptor electronic energy transfer: criteria to identify subsets of active normal modeses
dc.typeinfo:eu-repo/semantics/articlees
dspace.entity.typePublicationes
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