Real-Time Quantum Dynamics Reveals Complex, Many-Body Interactions in Solvated Nanodroplets

Autores
Oviedo, María Belén; Wong, Bryan M.
Año de publicación
2016
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
Electronic excitations in the liquid phase are surprisingly rich and considerably more complex than either gas-phase or solid-state systems. While the majority of physical and biological processes take place in solvent, our understanding of nonequilibrium excited-state processes in these condensed phase environments remains far from complete. A central and long-standing issue in these solvated environments is the assessment of many-body interactions, particularly when the entire system is out of equilibrium and many quantum states participate in the overall process. Here we present a microscopic picture of solute-solvent electron dynamics and solvatochromic effects, which we uncover using a new real-time quantum dynamics approach for extremely large solvated nanodroplets. In particular, we find that a complex interplay of quantum interactions underlies our observations of solute-solvent effects, and simple macroscopic solvatochromic shifts can even be qualitatively different at the microscopic molecular level in these systems. By treating both the solvent and the solute on the same footing at a quantum-mechanical level, we demonstrate that the electron dynamics in these systems are surprisingly complex, and the emergence of many-body interactions underlies the dynamics in these solvated systems.
Fil: Oviedo, María Belén. University Of California Riverside; Estados Unidos. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Fil: Wong, Bryan M.. University Of California Riverside; Estados Unidos
Materia
Dftb
Charge Transfer
Solar Cells
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:11336/50656

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spelling Real-Time Quantum Dynamics Reveals Complex, Many-Body Interactions in Solvated NanodropletsOviedo, María BelénWong, Bryan M.DftbCharge TransferSolar Cellshttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1Electronic excitations in the liquid phase are surprisingly rich and considerably more complex than either gas-phase or solid-state systems. While the majority of physical and biological processes take place in solvent, our understanding of nonequilibrium excited-state processes in these condensed phase environments remains far from complete. A central and long-standing issue in these solvated environments is the assessment of many-body interactions, particularly when the entire system is out of equilibrium and many quantum states participate in the overall process. Here we present a microscopic picture of solute-solvent electron dynamics and solvatochromic effects, which we uncover using a new real-time quantum dynamics approach for extremely large solvated nanodroplets. In particular, we find that a complex interplay of quantum interactions underlies our observations of solute-solvent effects, and simple macroscopic solvatochromic shifts can even be qualitatively different at the microscopic molecular level in these systems. By treating both the solvent and the solute on the same footing at a quantum-mechanical level, we demonstrate that the electron dynamics in these systems are surprisingly complex, and the emergence of many-body interactions underlies the dynamics in these solvated systems.Fil: Oviedo, María Belén. University Of California Riverside; Estados Unidos. Consejo Nacional de Investigaciones Científicas y Técnicas; ArgentinaFil: Wong, Bryan M.. University Of California Riverside; Estados UnidosAmerican Chemical Society2016-04-26info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/50656Oviedo, María Belén; Wong, Bryan M.; Real-Time Quantum Dynamics Reveals Complex, Many-Body Interactions in Solvated Nanodroplets; American Chemical Society; Journal of Chemical Theory and Computation; 12; 4; 26-4-2016; 1862-18711549-96181549-9626CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/https://pubs.acs.org/doi/10.1021/acs.jctc.5b01019info:eu-repo/semantics/altIdentifier/doi/10.1021/acs.jctc.5b01019info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-29T09:44:12Zoai:ri.conicet.gov.ar:11336/50656instacron: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:34982025-09-29 09:44:12.74CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Real-Time Quantum Dynamics Reveals Complex, Many-Body Interactions in Solvated Nanodroplets
title Real-Time Quantum Dynamics Reveals Complex, Many-Body Interactions in Solvated Nanodroplets
spellingShingle Real-Time Quantum Dynamics Reveals Complex, Many-Body Interactions in Solvated Nanodroplets
Oviedo, María Belén
Dftb
Charge Transfer
Solar Cells
title_short Real-Time Quantum Dynamics Reveals Complex, Many-Body Interactions in Solvated Nanodroplets
title_full Real-Time Quantum Dynamics Reveals Complex, Many-Body Interactions in Solvated Nanodroplets
title_fullStr Real-Time Quantum Dynamics Reveals Complex, Many-Body Interactions in Solvated Nanodroplets
title_full_unstemmed Real-Time Quantum Dynamics Reveals Complex, Many-Body Interactions in Solvated Nanodroplets
title_sort Real-Time Quantum Dynamics Reveals Complex, Many-Body Interactions in Solvated Nanodroplets
dc.creator.none.fl_str_mv Oviedo, María Belén
Wong, Bryan M.
author Oviedo, María Belén
author_facet Oviedo, María Belén
Wong, Bryan M.
author_role author
author2 Wong, Bryan M.
author2_role author
dc.subject.none.fl_str_mv Dftb
Charge Transfer
Solar Cells
topic Dftb
Charge Transfer
Solar Cells
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv Electronic excitations in the liquid phase are surprisingly rich and considerably more complex than either gas-phase or solid-state systems. While the majority of physical and biological processes take place in solvent, our understanding of nonequilibrium excited-state processes in these condensed phase environments remains far from complete. A central and long-standing issue in these solvated environments is the assessment of many-body interactions, particularly when the entire system is out of equilibrium and many quantum states participate in the overall process. Here we present a microscopic picture of solute-solvent electron dynamics and solvatochromic effects, which we uncover using a new real-time quantum dynamics approach for extremely large solvated nanodroplets. In particular, we find that a complex interplay of quantum interactions underlies our observations of solute-solvent effects, and simple macroscopic solvatochromic shifts can even be qualitatively different at the microscopic molecular level in these systems. By treating both the solvent and the solute on the same footing at a quantum-mechanical level, we demonstrate that the electron dynamics in these systems are surprisingly complex, and the emergence of many-body interactions underlies the dynamics in these solvated systems.
Fil: Oviedo, María Belén. University Of California Riverside; Estados Unidos. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Fil: Wong, Bryan M.. University Of California Riverside; Estados Unidos
description Electronic excitations in the liquid phase are surprisingly rich and considerably more complex than either gas-phase or solid-state systems. While the majority of physical and biological processes take place in solvent, our understanding of nonequilibrium excited-state processes in these condensed phase environments remains far from complete. A central and long-standing issue in these solvated environments is the assessment of many-body interactions, particularly when the entire system is out of equilibrium and many quantum states participate in the overall process. Here we present a microscopic picture of solute-solvent electron dynamics and solvatochromic effects, which we uncover using a new real-time quantum dynamics approach for extremely large solvated nanodroplets. In particular, we find that a complex interplay of quantum interactions underlies our observations of solute-solvent effects, and simple macroscopic solvatochromic shifts can even be qualitatively different at the microscopic molecular level in these systems. By treating both the solvent and the solute on the same footing at a quantum-mechanical level, we demonstrate that the electron dynamics in these systems are surprisingly complex, and the emergence of many-body interactions underlies the dynamics in these solvated systems.
publishDate 2016
dc.date.none.fl_str_mv 2016-04-26
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/11336/50656
Oviedo, María Belén; Wong, Bryan M.; Real-Time Quantum Dynamics Reveals Complex, Many-Body Interactions in Solvated Nanodroplets; American Chemical Society; Journal of Chemical Theory and Computation; 12; 4; 26-4-2016; 1862-1871
1549-9618
1549-9626
CONICET Digital
CONICET
url http://hdl.handle.net/11336/50656
identifier_str_mv Oviedo, María Belén; Wong, Bryan M.; Real-Time Quantum Dynamics Reveals Complex, Many-Body Interactions in Solvated Nanodroplets; American Chemical Society; Journal of Chemical Theory and Computation; 12; 4; 26-4-2016; 1862-1871
1549-9618
1549-9626
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/url/https://pubs.acs.org/doi/10.1021/acs.jctc.5b01019
info:eu-repo/semantics/altIdentifier/doi/10.1021/acs.jctc.5b01019
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 American Chemical Society
publisher.none.fl_str_mv American Chemical 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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