Non-adiabatic direct quantum dynamics using force fields: Toward solvation
Quantum dynamics simulations are becoming a powerful tool for understanding photo-excited molecules. Their poor scaling, however, means that it is hard to study molecules with more than a few atoms accurately, and a major challenge at the moment is the inclusion of the molecular environment. Here, w...
| Autores: | , , , , , , , |
|---|---|
| Tipo de recurso: | artículo |
| Fecha de publicación: | 2024 |
| País: | España |
| Institución: | Universidad Autónoma de Madrid |
| Repositorio: | Biblos-e Archivo. Repositorio Institucional de la UAM |
| Idioma: | inglés |
| OAI Identifier: | oai:repositorio.uam.es:10486/716591 |
| Acceso en línea: | http://hdl.handle.net/10486/716591 https://dx.doi.org/10.1063/5.0204911 |
| Access Level: | acceso abierto |
| Palabra clave: | Degrees of freedom (mechanics) dynamics potential energy potential energy surfaces quantum chemistry Química |
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Non-adiabatic direct quantum dynamics using force fields: Toward solvationCigrang, LeónGreen, J.A.Gómez, SandraCerezo Bastida, JavierImprota, RobertoPrampolini, GiacomoSantoro, FabrizioWorth, Graham A.Degrees of freedom (mechanics)dynamicspotential energypotential energy surfacesquantum chemistryQuímicaQuantum dynamics simulations are becoming a powerful tool for understanding photo-excited molecules. Their poor scaling, however, means that it is hard to study molecules with more than a few atoms accurately, and a major challenge at the moment is the inclusion of the molecular environment. Here, we present a proof of principle for a way to break the two bottlenecks preventing large but accurate simulations. First, the problem of providing the potential energy surfaces for a general system is addressed by parameterizing a standard force field to reproduce the potential surfaces of the molecule’s excited-states, including the all-important vibronic coupling. While not shown here, this would trivially enable the use of an explicit solvent. Second, to help the scaling of the nuclear dynamics propagation, a hierarchy of approximations is introduced to the variational multi-configurational Gaussian method that retains the variational quantum wavepacket description of the key quantum degrees of freedom and uses classical trajectories for the remaining in a quantum mechanics/molecular mechanics like approach. The method is referred to as force field quantum dynamics (FF-QD), and a two-state ππ*/nπ* model of uracil, excited to its lowest bright ππ* state, is used as a test caseThe research in this paper was a result of an exchange program funded by the Royal Society (Grant No. IEC/R2/202236) and the CNR (Bilaterale Grant No. CNR-RSC 2021). R.I., G.P., and F.S. also thank the CNR program “Progetti di Ricerca @ cnr,” Project No. UCATG4, and R.I. also acknowledges the financial support through Grant No. NUTRAGE FOE-2021 DBA.AD005.225. F.S. and G.P. also thank the ICSC - Centro Nazionale di Richercha in High Performance Computing, Big Data and Quantum Computing, funded by the Next Generation EU - PNRR, Missione 4 Componente 2 Investimento 1.4. S.G. acknowledges the María Zambrano grant (NextGenEU funds), the USAL grant “Programa Propio C1,” and the funding by the Spanish Ministry of Science and Innovation (MCIN/AEI/10.13039/501100011033), Grant No. PID2020-113147GA-I00. The work has also been supported in the UK by the EPSRC under Grant No. EP/V026690/1. J.A.G. gratefully acknowledges the current funding of a research fellowship by the Alexander von Humboldt FoundationAmerican Institute of PhysicsDepartamento de QuímicaFacultad de Ciencias20242024-05-07research articlehttp://purl.org/coar/resource_type/c_2df8fbb1VoRhttp://purl.org/coar/version/c_970fb48d4fbd8a85info:eu-repo/semantics/articleapplication/pdfhttp://hdl.handle.net/10486/716591https://dx.doi.org/10.1063/5.0204911reponame:Biblos-e Archivo. Repositorio Institucional de la UAMinstname:Universidad Autónoma de MadridInglésengopen accesshttp://purl.org/coar/access_right/c_abf2Attribution 4.0 Internationalhttp://creativecommons.org/licenses/by/4.0/info:eu-repo/semantics/openAccessoai:repositorio.uam.es:10486/7165912026-06-23T12:46:27Z |
| dc.title.none.fl_str_mv |
Non-adiabatic direct quantum dynamics using force fields: Toward solvation |
| title |
Non-adiabatic direct quantum dynamics using force fields: Toward solvation |
| spellingShingle |
Non-adiabatic direct quantum dynamics using force fields: Toward solvation Cigrang, León Degrees of freedom (mechanics) dynamics potential energy potential energy surfaces quantum chemistry Química |
| title_short |
Non-adiabatic direct quantum dynamics using force fields: Toward solvation |
| title_full |
Non-adiabatic direct quantum dynamics using force fields: Toward solvation |
| title_fullStr |
Non-adiabatic direct quantum dynamics using force fields: Toward solvation |
| title_full_unstemmed |
Non-adiabatic direct quantum dynamics using force fields: Toward solvation |
| title_sort |
Non-adiabatic direct quantum dynamics using force fields: Toward solvation |
| dc.creator.none.fl_str_mv |
Cigrang, León Green, J.A. Gómez, Sandra Cerezo Bastida, Javier Improta, Roberto Prampolini, Giacomo Santoro, Fabrizio Worth, Graham A. |
| author |
Cigrang, León |
| author_facet |
Cigrang, León Green, J.A. Gómez, Sandra Cerezo Bastida, Javier Improta, Roberto Prampolini, Giacomo Santoro, Fabrizio Worth, Graham A. |
| author_role |
author |
| author2 |
Green, J.A. Gómez, Sandra Cerezo Bastida, Javier Improta, Roberto Prampolini, Giacomo Santoro, Fabrizio Worth, Graham A. |
| author2_role |
author author author author author author author |
| dc.contributor.none.fl_str_mv |
Departamento de Química Facultad de Ciencias |
| dc.subject.none.fl_str_mv |
Degrees of freedom (mechanics) dynamics potential energy potential energy surfaces quantum chemistry Química |
| topic |
Degrees of freedom (mechanics) dynamics potential energy potential energy surfaces quantum chemistry Química |
| description |
Quantum dynamics simulations are becoming a powerful tool for understanding photo-excited molecules. Their poor scaling, however, means that it is hard to study molecules with more than a few atoms accurately, and a major challenge at the moment is the inclusion of the molecular environment. Here, we present a proof of principle for a way to break the two bottlenecks preventing large but accurate simulations. First, the problem of providing the potential energy surfaces for a general system is addressed by parameterizing a standard force field to reproduce the potential surfaces of the molecule’s excited-states, including the all-important vibronic coupling. While not shown here, this would trivially enable the use of an explicit solvent. Second, to help the scaling of the nuclear dynamics propagation, a hierarchy of approximations is introduced to the variational multi-configurational Gaussian method that retains the variational quantum wavepacket description of the key quantum degrees of freedom and uses classical trajectories for the remaining in a quantum mechanics/molecular mechanics like approach. The method is referred to as force field quantum dynamics (FF-QD), and a two-state ππ*/nπ* model of uracil, excited to its lowest bright ππ* state, is used as a test case |
| publishDate |
2024 |
| dc.date.none.fl_str_mv |
2024 2024-05-07 |
| 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/10486/716591 https://dx.doi.org/10.1063/5.0204911 |
| url |
http://hdl.handle.net/10486/716591 https://dx.doi.org/10.1063/5.0204911 |
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Inglés eng |
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Inglés |
| language |
eng |
| dc.rights.none.fl_str_mv |
open access http://purl.org/coar/access_right/c_abf2 Attribution 4.0 International http://creativecommons.org/licenses/by/4.0/ |
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info:eu-repo/semantics/openAccess |
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open access http://purl.org/coar/access_right/c_abf2 Attribution 4.0 International http://creativecommons.org/licenses/by/4.0/ |
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openAccess |
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application/pdf |
| dc.publisher.none.fl_str_mv |
American Institute of Physics |
| publisher.none.fl_str_mv |
American Institute of Physics |
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reponame:Biblos-e Archivo. Repositorio Institucional de la UAM instname:Universidad Autónoma de Madrid |
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Universidad Autónoma de Madrid |
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Biblos-e Archivo. Repositorio Institucional de la UAM |
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Biblos-e Archivo. Repositorio Institucional de la UAM |
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