Mixed Quantum/Classical Method for Nonadiabatic Quantum Dynamics in Explicit Solvent Models: The ππ∗/nπ∗ Decay of Thymine in Water as a Test Case

We present a novel mixed quantum classical dynamical method to include solvent effects on internal conversion (IC) processes. All the solute degrees of freedom are represented by a wavepacket moving according to nonadiabatic quantum dynamics, while the motion of an explicit solvent model is describe...

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Detalles Bibliográficos
Autores: Cerezo Bastida, Javier, Liu, Yanli, Lin, Na, Zhao, Xian, Improta, Roberto, Santoro, Fabrizio
Tipo de recurso: artículo
Fecha de publicación:2018
País:España
Institución:Universidad Autónoma de Madrid
Repositorio:Biblos-e Archivo. Repositorio Institucional de la UAM
Idioma:inglés
OAI Identifier:oai:repositorio.uam.es:10486/710377
Acceso en línea:http://hdl.handle.net/10486/710377
https://dx.doi.org/10.1021/acs.jctc.7b01015
Access Level:acceso abierto
Palabra clave:Thymine
DNA
Nucleobases
Química
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spelling Mixed Quantum/Classical Method for Nonadiabatic Quantum Dynamics in Explicit Solvent Models: The ππ∗/nπ∗ Decay of Thymine in Water as a Test CaseCerezo Bastida, JavierLiu, YanliLin, NaZhao, XianImprota, RobertoSantoro, FabrizioThymineDNANucleobasesQuímicaWe present a novel mixed quantum classical dynamical method to include solvent effects on internal conversion (IC) processes. All the solute degrees of freedom are represented by a wavepacket moving according to nonadiabatic quantum dynamics, while the motion of an explicit solvent model is described by an ensemble of classical trajectories. The mutual coupling of the solute and solvent dynamics is included within a mean-field framework and the quantum and classical equations of motions are solved simultaneously. As a test case we apply our method to the ultrafast ππ∗ → nπ∗ decay of thymine in water. Solvent dynamical response modifies IC yield already on the 50 fs time scale. This effect is due to water librational motions that stabilize the most populated state. Pure static disorder, that is, the existence of different solvent configurations when photoexcitation takes place, also has a remarkable impact on the dynamicsThe support of MIUR (PRIN 2010-2011 prot. 2010ERFKXL) is acknowledged. J.C. acknowledges the Fundacioń Ramoń Areces for funding his Postdoctoral position in Pisa and the fellowship provided by “Fundacioń Seńeca − Agencia de Ciencia y Tecnología de la Regioń de Murcia” through the “Saavedra-Fajardo” program (20028/SF/16). R.I. thanks the Université Paris-Saclay (Chaire d’Alembert No. 2016-10751). Y. L. acknowledges the financial support from the China Scholarship Council (CSC, No. 201506220064) and Y.L. and N. L. a generous grant of computer time from the Norwegian Programme for Supercomputing. N. L. also acknowledges the National Nature Science Foundation of China (Grant No. 21573129). The authors gratefully acknowledge G. Worth for making available the Quantics code and for useful discussionsAmerican Chemical SocietyDepartamento de Química Física AplicadaFacultad de Ciencias20182018-02-13research articlehttp://purl.org/coar/resource_type/c_2df8fbb1VoRhttp://purl.org/coar/version/c_970fb48d4fbd8a85info:eu-repo/semantics/articleapplication/pdfhttp://hdl.handle.net/10486/710377https://dx.doi.org/10.1021/acs.jctc.7b01015reponame:Biblos-e Archivo. Repositorio Institucional de la UAMinstname:Universidad Autónoma de MadridInglésengopen accesshttp://purl.org/coar/access_right/c_abf2info:eu-repo/semantics/openAccessoai:repositorio.uam.es:10486/7103772026-06-23T12:46:27Z
dc.title.none.fl_str_mv Mixed Quantum/Classical Method for Nonadiabatic Quantum Dynamics in Explicit Solvent Models: The ππ∗/nπ∗ Decay of Thymine in Water as a Test Case
title Mixed Quantum/Classical Method for Nonadiabatic Quantum Dynamics in Explicit Solvent Models: The ππ∗/nπ∗ Decay of Thymine in Water as a Test Case
spellingShingle Mixed Quantum/Classical Method for Nonadiabatic Quantum Dynamics in Explicit Solvent Models: The ππ∗/nπ∗ Decay of Thymine in Water as a Test Case
Cerezo Bastida, Javier
Thymine
DNA
Nucleobases
Química
title_short Mixed Quantum/Classical Method for Nonadiabatic Quantum Dynamics in Explicit Solvent Models: The ππ∗/nπ∗ Decay of Thymine in Water as a Test Case
title_full Mixed Quantum/Classical Method for Nonadiabatic Quantum Dynamics in Explicit Solvent Models: The ππ∗/nπ∗ Decay of Thymine in Water as a Test Case
title_fullStr Mixed Quantum/Classical Method for Nonadiabatic Quantum Dynamics in Explicit Solvent Models: The ππ∗/nπ∗ Decay of Thymine in Water as a Test Case
title_full_unstemmed Mixed Quantum/Classical Method for Nonadiabatic Quantum Dynamics in Explicit Solvent Models: The ππ∗/nπ∗ Decay of Thymine in Water as a Test Case
title_sort Mixed Quantum/Classical Method for Nonadiabatic Quantum Dynamics in Explicit Solvent Models: The ππ∗/nπ∗ Decay of Thymine in Water as a Test Case
dc.creator.none.fl_str_mv Cerezo Bastida, Javier
Liu, Yanli
Lin, Na
Zhao, Xian
Improta, Roberto
Santoro, Fabrizio
author Cerezo Bastida, Javier
author_facet Cerezo Bastida, Javier
Liu, Yanli
Lin, Na
Zhao, Xian
Improta, Roberto
Santoro, Fabrizio
author_role author
author2 Liu, Yanli
Lin, Na
Zhao, Xian
Improta, Roberto
Santoro, Fabrizio
author2_role author
author
author
author
author
dc.contributor.none.fl_str_mv Departamento de Química Física Aplicada
Facultad de Ciencias
dc.subject.none.fl_str_mv Thymine
DNA
Nucleobases
Química
topic Thymine
DNA
Nucleobases
Química
description We present a novel mixed quantum classical dynamical method to include solvent effects on internal conversion (IC) processes. All the solute degrees of freedom are represented by a wavepacket moving according to nonadiabatic quantum dynamics, while the motion of an explicit solvent model is described by an ensemble of classical trajectories. The mutual coupling of the solute and solvent dynamics is included within a mean-field framework and the quantum and classical equations of motions are solved simultaneously. As a test case we apply our method to the ultrafast ππ∗ → nπ∗ decay of thymine in water. Solvent dynamical response modifies IC yield already on the 50 fs time scale. This effect is due to water librational motions that stabilize the most populated state. Pure static disorder, that is, the existence of different solvent configurations when photoexcitation takes place, also has a remarkable impact on the dynamics
publishDate 2018
dc.date.none.fl_str_mv 2018
2018-02-13
dc.type.none.fl_str_mv research article
http://purl.org/coar/resource_type/c_2df8fbb1
VoR
http://purl.org/coar/version/c_970fb48d4fbd8a85
dc.type.openaire.fl_str_mv info:eu-repo/semantics/article
format article
dc.identifier.none.fl_str_mv http://hdl.handle.net/10486/710377
https://dx.doi.org/10.1021/acs.jctc.7b01015
url http://hdl.handle.net/10486/710377
https://dx.doi.org/10.1021/acs.jctc.7b01015
dc.language.none.fl_str_mv Inglés
eng
language_invalid_str_mv Inglés
language eng
dc.rights.none.fl_str_mv open access
http://purl.org/coar/access_right/c_abf2
dc.rights.openaire.fl_str_mv info:eu-repo/semantics/openAccess
rights_invalid_str_mv open access
http://purl.org/coar/access_right/c_abf2
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
dc.publisher.none.fl_str_mv American Chemical Society
publisher.none.fl_str_mv American Chemical Society
dc.source.none.fl_str_mv reponame:Biblos-e Archivo. Repositorio Institucional de la UAM
instname:Universidad Autónoma de Madrid
instname_str Universidad Autónoma de Madrid
reponame_str Biblos-e Archivo. Repositorio Institucional de la UAM
collection Biblos-e Archivo. Repositorio Institucional de la UAM
repository.name.fl_str_mv
repository.mail.fl_str_mv
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