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
- Institución
- Consejo Nacional de Investigaciones Científicas y Técnicas
- OAI Identificador
- oai:ri.conicet.gov.ar:11336/50656
Ver los metadatos del registro completo
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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 |
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CONICET Digital (CONICET) |
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CONICET Digital (CONICET) |
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Consejo Nacional de Investigaciones Científicas y Técnicas |
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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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13.070432 |