Radiative thermalization in semiclassical simulations of light-matter interaction

Autores
Gadea, Esteban David; Bustamante, Carlos Mauricio; Todorov, Tchavdar N.; Scherlis Perel, Damian Ariel
Año de publicación
2022
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
Prediction of the equilibrium populations in quantum dynamics simulations of molecules exposed to black-body radiation has proved challenging for semiclassical treatments, with the usual Ehrenfest and Maxwell-Bloch methods exhibiting serious failures. In this context, we explore the behavior of a recently introduced semiclassical model of light-matter interaction derived from a dissipative Lagrangian [C. M. Bustamante, E. D. Gadea, A. Horsfield, T. N. Todorov, M. C. González Lebrero, and D. A. Scherlis, Phys. Rev. Lett. 126, 087401 (2021)0031-900710.1103/PhysRevLett.126.087401]. It is shown that this model reproduces the Boltzmann populations for two-level systems, predicting the black-body spectra in approximate agreement with Planck's distribution. In multilevel systems, small deviations from the expected occupations are seen beyond the first excited level. By averaging over fast oscillations, a rate equation is derived from the dissipative equation of motion that makes it possible to rationalize these deviations. Importantly, it enables us to conclude that this model will produce the correct equilibrium populations provided the occupations of the lowest levels remain close to unity, a condition satisfied at low temperature or small excitations.
Fil: Gadea, Esteban David. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de los Materiales, Medioambiente y Energía. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Instituto de Química, Física de los Materiales, Medioambiente y Energía; Argentina
Fil: Bustamante, Carlos Mauricio. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de los Materiales, Medioambiente y Energía. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Instituto de Química, Física de los Materiales, Medioambiente y Energía; Argentina
Fil: Todorov, Tchavdar N.. The Queens University of Belfast; Irlanda
Fil: Scherlis Perel, Damian Ariel. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de los Materiales, Medioambiente y Energía. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Instituto de Química, Física de los Materiales, Medioambiente y Energía; Argentina
Materia
Thermalization
Radiation
Light-matter interaction
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:11336/210128
Acceder
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spelling Radiative thermalization in semiclassical simulations of light-matter interactionGadea, Esteban DavidBustamante, Carlos MauricioTodorov, Tchavdar N.Scherlis Perel, Damian ArielThermalizationRadiationLight-matter interactionhttps://purl.org/becyt/ford/1.3https://purl.org/becyt/ford/1Prediction of the equilibrium populations in quantum dynamics simulations of molecules exposed to black-body radiation has proved challenging for semiclassical treatments, with the usual Ehrenfest and Maxwell-Bloch methods exhibiting serious failures. In this context, we explore the behavior of a recently introduced semiclassical model of light-matter interaction derived from a dissipative Lagrangian [C. M. Bustamante, E. D. Gadea, A. Horsfield, T. N. Todorov, M. C. González Lebrero, and D. A. Scherlis, Phys. Rev. Lett. 126, 087401 (2021)0031-900710.1103/PhysRevLett.126.087401]. It is shown that this model reproduces the Boltzmann populations for two-level systems, predicting the black-body spectra in approximate agreement with Planck's distribution. In multilevel systems, small deviations from the expected occupations are seen beyond the first excited level. By averaging over fast oscillations, a rate equation is derived from the dissipative equation of motion that makes it possible to rationalize these deviations. Importantly, it enables us to conclude that this model will produce the correct equilibrium populations provided the occupations of the lowest levels remain close to unity, a condition satisfied at low temperature or small excitations.Fil: Gadea, Esteban David. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de los Materiales, Medioambiente y Energía. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Instituto de Química, Física de los Materiales, Medioambiente y Energía; ArgentinaFil: Bustamante, Carlos Mauricio. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de los Materiales, Medioambiente y Energía. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Instituto de Química, Física de los Materiales, Medioambiente y Energía; ArgentinaFil: Todorov, Tchavdar N.. The Queens University of Belfast; IrlandaFil: Scherlis Perel, Damian Ariel. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de los Materiales, Medioambiente y Energía. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Instituto de Química, Física de los Materiales, Medioambiente y Energía; ArgentinaAmerican Physical Society2022-04info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfapplication/pdfapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/210128Gadea, Esteban David; Bustamante, Carlos Mauricio; Todorov, Tchavdar N.; Scherlis Perel, Damian Ariel; Radiative thermalization in semiclassical simulations of light-matter interaction; American Physical Society; Physical Review A; 105; 4; 4-2022; 1-102469-99262469-9934CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/doi/10.1103/PhysRevA.105.042201info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-10-15T15:39:29Zoai:ri.conicet.gov.ar:11336/210128instacron: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:34982025-10-15 15:39:29.558CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Radiative thermalization in semiclassical simulations of light-matter interaction
title Radiative thermalization in semiclassical simulations of light-matter interaction
spellingShingle Radiative thermalization in semiclassical simulations of light-matter interaction
Gadea, Esteban David
Thermalization
Radiation
Light-matter interaction
title_short Radiative thermalization in semiclassical simulations of light-matter interaction
title_full Radiative thermalization in semiclassical simulations of light-matter interaction
title_fullStr Radiative thermalization in semiclassical simulations of light-matter interaction
title_full_unstemmed Radiative thermalization in semiclassical simulations of light-matter interaction
title_sort Radiative thermalization in semiclassical simulations of light-matter interaction
dc.creator.none.fl_str_mv Gadea, Esteban David
Bustamante, Carlos Mauricio
Todorov, Tchavdar N.
Scherlis Perel, Damian Ariel
author Gadea, Esteban David
author_facet Gadea, Esteban David
Bustamante, Carlos Mauricio
Todorov, Tchavdar N.
Scherlis Perel, Damian Ariel
author_role author
author2 Bustamante, Carlos Mauricio
Todorov, Tchavdar N.
Scherlis Perel, Damian Ariel
author2_role author
author
author
dc.subject.none.fl_str_mv Thermalization
Radiation
Light-matter interaction
topic Thermalization
Radiation
Light-matter interaction
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.3
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv Prediction of the equilibrium populations in quantum dynamics simulations of molecules exposed to black-body radiation has proved challenging for semiclassical treatments, with the usual Ehrenfest and Maxwell-Bloch methods exhibiting serious failures. In this context, we explore the behavior of a recently introduced semiclassical model of light-matter interaction derived from a dissipative Lagrangian [C. M. Bustamante, E. D. Gadea, A. Horsfield, T. N. Todorov, M. C. González Lebrero, and D. A. Scherlis, Phys. Rev. Lett. 126, 087401 (2021)0031-900710.1103/PhysRevLett.126.087401]. It is shown that this model reproduces the Boltzmann populations for two-level systems, predicting the black-body spectra in approximate agreement with Planck's distribution. In multilevel systems, small deviations from the expected occupations are seen beyond the first excited level. By averaging over fast oscillations, a rate equation is derived from the dissipative equation of motion that makes it possible to rationalize these deviations. Importantly, it enables us to conclude that this model will produce the correct equilibrium populations provided the occupations of the lowest levels remain close to unity, a condition satisfied at low temperature or small excitations.
Fil: Gadea, Esteban David. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de los Materiales, Medioambiente y Energía. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Instituto de Química, Física de los Materiales, Medioambiente y Energía; Argentina
Fil: Bustamante, Carlos Mauricio. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de los Materiales, Medioambiente y Energía. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Instituto de Química, Física de los Materiales, Medioambiente y Energía; Argentina
Fil: Todorov, Tchavdar N.. The Queens University of Belfast; Irlanda
Fil: Scherlis Perel, Damian Ariel. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de los Materiales, Medioambiente y Energía. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Instituto de Química, Física de los Materiales, Medioambiente y Energía; Argentina
description Prediction of the equilibrium populations in quantum dynamics simulations of molecules exposed to black-body radiation has proved challenging for semiclassical treatments, with the usual Ehrenfest and Maxwell-Bloch methods exhibiting serious failures. In this context, we explore the behavior of a recently introduced semiclassical model of light-matter interaction derived from a dissipative Lagrangian [C. M. Bustamante, E. D. Gadea, A. Horsfield, T. N. Todorov, M. C. González Lebrero, and D. A. Scherlis, Phys. Rev. Lett. 126, 087401 (2021)0031-900710.1103/PhysRevLett.126.087401]. It is shown that this model reproduces the Boltzmann populations for two-level systems, predicting the black-body spectra in approximate agreement with Planck's distribution. In multilevel systems, small deviations from the expected occupations are seen beyond the first excited level. By averaging over fast oscillations, a rate equation is derived from the dissipative equation of motion that makes it possible to rationalize these deviations. Importantly, it enables us to conclude that this model will produce the correct equilibrium populations provided the occupations of the lowest levels remain close to unity, a condition satisfied at low temperature or small excitations.
publishDate 2022
dc.date.none.fl_str_mv 2022-04
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/11336/210128
Gadea, Esteban David; Bustamante, Carlos Mauricio; Todorov, Tchavdar N.; Scherlis Perel, Damian Ariel; Radiative thermalization in semiclassical simulations of light-matter interaction; American Physical Society; Physical Review A; 105; 4; 4-2022; 1-10
2469-9926
2469-9934
CONICET Digital
CONICET
url http://hdl.handle.net/11336/210128
identifier_str_mv Gadea, Esteban David; Bustamante, Carlos Mauricio; Todorov, Tchavdar N.; Scherlis Perel, Damian Ariel; Radiative thermalization in semiclassical simulations of light-matter interaction; American Physical Society; Physical Review A; 105; 4; 4-2022; 1-10
2469-9926
2469-9934
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/doi/10.1103/PhysRevA.105.042201
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
application/pdf
application/pdf
application/pdf
dc.publisher.none.fl_str_mv American Physical Society
publisher.none.fl_str_mv American Physical Society
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 13.22299

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