Nonadiabatic excited-state molecular dynamics: On-the-fly limiting of essential excited states

Autores
Nelson, Tammie; Naumov, Artem; Fernández Alberti, Sebastián; Tretiak, Sergei
Año de publicación
2016
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
The simulation of nonadiabatic dynamics in extended molecular systems involving hundreds of atoms and large densities of states is particularly challenging. Nonadiabatic coupling terms (NACTs) represent a significant numerical bottleneck in surface hopping approaches. Rather than using unreliable NACT cutting schemes, here we develop “on-the-fly” state limiting methods to eliminate states that are no longer essential for the non-radiative relaxation dynamics as a trajectory proceeds. We propose a state number criteria and an energy-based state limit. The latter is more physically relevant by requiring a user-imposed energy threshold. For this purpose, we introduce a local kinetic energy gauge by summing contributions from atoms within the spatial localization of the electronic wavefunction to define the energy available for upward hops. The proposed state limiting schemes are implemented within the nonadiabatic excited-state molecular dynamics framework to simulate photoinduced relaxation in poly-phenylene vinylene (PPV) and branched poly-phenylene ethynylene (PPE) oligomers for benchmark evaluation.
Fil: Nelson, Tammie. Los Alamos National Laboratory; Estados Unidos
Fil: Naumov, Artem. Skolkovo Institute Of Science And Technology; Rusia
Fil: Fernández Alberti, Sebastián. Universidad Nacional de Quilmes; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Fil: Tretiak, Sergei. Los Alamos National Laboratory; Estados Unidos
Materia
Excited State Limiting
Fewest Switches Surface Hopping
Local Kinetic Energy
Na-Esmd
Poly-Phenylene Ethynylene
Poly-Phenylene Vinylene
Nivel de accesibilidad
acceso abierto
Condiciones de uso
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
Repositorio
CONICET Digital (CONICET)
Institución
Consejo Nacional de Investigaciones Científicas y Técnicas
OAI Identificador
oai:ri.conicet.gov.ar:11336/38564
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/38564
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Nonadiabatic excited-state molecular dynamics: On-the-fly limiting of essential excited statesNelson, TammieNaumov, ArtemFernández Alberti, SebastiánTretiak, SergeiExcited State LimitingFewest Switches Surface HoppingLocal Kinetic EnergyNa-EsmdPoly-Phenylene EthynylenePoly-Phenylene Vinylenehttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1The simulation of nonadiabatic dynamics in extended molecular systems involving hundreds of atoms and large densities of states is particularly challenging. Nonadiabatic coupling terms (NACTs) represent a significant numerical bottleneck in surface hopping approaches. Rather than using unreliable NACT cutting schemes, here we develop “on-the-fly” state limiting methods to eliminate states that are no longer essential for the non-radiative relaxation dynamics as a trajectory proceeds. We propose a state number criteria and an energy-based state limit. The latter is more physically relevant by requiring a user-imposed energy threshold. For this purpose, we introduce a local kinetic energy gauge by summing contributions from atoms within the spatial localization of the electronic wavefunction to define the energy available for upward hops. The proposed state limiting schemes are implemented within the nonadiabatic excited-state molecular dynamics framework to simulate photoinduced relaxation in poly-phenylene vinylene (PPV) and branched poly-phenylene ethynylene (PPE) oligomers for benchmark evaluation.Fil: Nelson, Tammie. Los Alamos National Laboratory; Estados UnidosFil: Naumov, Artem. Skolkovo Institute Of Science And Technology; RusiaFil: Fernández Alberti, Sebastián. Universidad Nacional de Quilmes; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; ArgentinaFil: Tretiak, Sergei. Los Alamos National Laboratory; Estados UnidosElsevier Science2016-12info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/38564Nelson, Tammie; Naumov, Artem; Fernández Alberti, Sebastián; Tretiak, Sergei; Nonadiabatic excited-state molecular dynamics: On-the-fly limiting of essential excited states; Elsevier Science; Chemical Physics; 481; 12-2016; 84-900301-0104CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/doi/10.1016/j.chemphys.2016.05.017info:eu-repo/semantics/altIdentifier/url/https://www.sciencedirect.com/science/article/pii/S0301010416301914info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-10T13:03:38Zoai:ri.conicet.gov.ar:11336/38564instacron:CONICETInstitucionalhttp://ri.conicet.gov.ar/Organismo científico-tecnológicoNo correspondehttp://ri.conicet.gov.ar/oai/requestdasensio@conicet.gov.ar; lcarlino@conicet.gov.arArgentinaNo correspondeNo correspondeNo correspondeopendoar:34982025-09-10 13:03:38.861CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Nonadiabatic excited-state molecular dynamics: On-the-fly limiting of essential excited states
title Nonadiabatic excited-state molecular dynamics: On-the-fly limiting of essential excited states
spellingShingle Nonadiabatic excited-state molecular dynamics: On-the-fly limiting of essential excited states
Nelson, Tammie
Excited State Limiting
Fewest Switches Surface Hopping
Local Kinetic Energy
Na-Esmd
Poly-Phenylene Ethynylene
Poly-Phenylene Vinylene
title_short Nonadiabatic excited-state molecular dynamics: On-the-fly limiting of essential excited states
title_full Nonadiabatic excited-state molecular dynamics: On-the-fly limiting of essential excited states
title_fullStr Nonadiabatic excited-state molecular dynamics: On-the-fly limiting of essential excited states
title_full_unstemmed Nonadiabatic excited-state molecular dynamics: On-the-fly limiting of essential excited states
title_sort Nonadiabatic excited-state molecular dynamics: On-the-fly limiting of essential excited states
dc.creator.none.fl_str_mv Nelson, Tammie
Naumov, Artem
Fernández Alberti, Sebastián
Tretiak, Sergei
author Nelson, Tammie
author_facet Nelson, Tammie
Naumov, Artem
Fernández Alberti, Sebastián
Tretiak, Sergei
author_role author
author2 Naumov, Artem
Fernández Alberti, Sebastián
Tretiak, Sergei
author2_role author
author
author
dc.subject.none.fl_str_mv Excited State Limiting
Fewest Switches Surface Hopping
Local Kinetic Energy
Na-Esmd
Poly-Phenylene Ethynylene
Poly-Phenylene Vinylene
topic Excited State Limiting
Fewest Switches Surface Hopping
Local Kinetic Energy
Na-Esmd
Poly-Phenylene Ethynylene
Poly-Phenylene Vinylene
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv The simulation of nonadiabatic dynamics in extended molecular systems involving hundreds of atoms and large densities of states is particularly challenging. Nonadiabatic coupling terms (NACTs) represent a significant numerical bottleneck in surface hopping approaches. Rather than using unreliable NACT cutting schemes, here we develop “on-the-fly” state limiting methods to eliminate states that are no longer essential for the non-radiative relaxation dynamics as a trajectory proceeds. We propose a state number criteria and an energy-based state limit. The latter is more physically relevant by requiring a user-imposed energy threshold. For this purpose, we introduce a local kinetic energy gauge by summing contributions from atoms within the spatial localization of the electronic wavefunction to define the energy available for upward hops. The proposed state limiting schemes are implemented within the nonadiabatic excited-state molecular dynamics framework to simulate photoinduced relaxation in poly-phenylene vinylene (PPV) and branched poly-phenylene ethynylene (PPE) oligomers for benchmark evaluation.
Fil: Nelson, Tammie. Los Alamos National Laboratory; Estados Unidos
Fil: Naumov, Artem. Skolkovo Institute Of Science And Technology; Rusia
Fil: Fernández Alberti, Sebastián. Universidad Nacional de Quilmes; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Fil: Tretiak, Sergei. Los Alamos National Laboratory; Estados Unidos
description The simulation of nonadiabatic dynamics in extended molecular systems involving hundreds of atoms and large densities of states is particularly challenging. Nonadiabatic coupling terms (NACTs) represent a significant numerical bottleneck in surface hopping approaches. Rather than using unreliable NACT cutting schemes, here we develop “on-the-fly” state limiting methods to eliminate states that are no longer essential for the non-radiative relaxation dynamics as a trajectory proceeds. We propose a state number criteria and an energy-based state limit. The latter is more physically relevant by requiring a user-imposed energy threshold. For this purpose, we introduce a local kinetic energy gauge by summing contributions from atoms within the spatial localization of the electronic wavefunction to define the energy available for upward hops. The proposed state limiting schemes are implemented within the nonadiabatic excited-state molecular dynamics framework to simulate photoinduced relaxation in poly-phenylene vinylene (PPV) and branched poly-phenylene ethynylene (PPE) oligomers for benchmark evaluation.
publishDate 2016
dc.date.none.fl_str_mv 2016-12
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/publishedVersion
http://purl.org/coar/resource_type/c_6501
info:ar-repo/semantics/articulo
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/11336/38564
Nelson, Tammie; Naumov, Artem; Fernández Alberti, Sebastián; Tretiak, Sergei; Nonadiabatic excited-state molecular dynamics: On-the-fly limiting of essential excited states; Elsevier Science; Chemical Physics; 481; 12-2016; 84-90
0301-0104
CONICET Digital
CONICET
url http://hdl.handle.net/11336/38564
identifier_str_mv Nelson, Tammie; Naumov, Artem; Fernández Alberti, Sebastián; Tretiak, Sergei; Nonadiabatic excited-state molecular dynamics: On-the-fly limiting of essential excited states; Elsevier Science; Chemical Physics; 481; 12-2016; 84-90
0301-0104
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/doi/10.1016/j.chemphys.2016.05.017
info:eu-repo/semantics/altIdentifier/url/https://www.sciencedirect.com/science/article/pii/S0301010416301914
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
eu_rights_str_mv openAccess
rights_invalid_str_mv https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
dc.format.none.fl_str_mv application/pdf
application/pdf
dc.publisher.none.fl_str_mv Elsevier Science
publisher.none.fl_str_mv Elsevier Science
dc.source.none.fl_str_mv reponame:CONICET Digital (CONICET)
instname:Consejo Nacional de Investigaciones Científicas y Técnicas
reponame_str CONICET Digital (CONICET)
collection CONICET Digital (CONICET)
instname_str Consejo Nacional de Investigaciones Científicas y Técnicas
repository.name.fl_str_mv CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicas
repository.mail.fl_str_mv dasensio@conicet.gov.ar; lcarlino@conicet.gov.ar
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score 12.993085

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