Real-time quantum dynamics of long-range electronic excitation transfer in plasmonic nanoantennas

Autores
Ilawe, Niranjan V.; Oviedo, María Belén; Wong, Bryan M.
Año de publicación
2017
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
Using large-scale, real-time, quantum dynamics calculations, we present a detailed analysis of electronic excitation transfer (EET) mechanisms in a multiparticle plasmonic nanoantenna system. Specifically, we utilize real-time, time-dependent, density functional tight binding (RT-TDDFTB) to provide a quantum-mechanical description (at an electronic/atomistic level of detail) for characterizing and analyzing these systems, without recourse to classical approximations. We also demonstrate highly long-range electronic couplings in these complex systems and find that the range of these couplings is more than twice the conventional cutoff limit considered by Förster resonance energy transfer (FRET)-based approaches. Furthermore, we attribute these unusually long-ranged electronic couplings to the coherent oscillations of conduction electrons in plasmonic nanoparticles. This long-range nature of plasmonic interactions has important ramifications for EET; in particular, we show that the commonly used "nearest-neighbor" FRET model is inadequate for accurately characterizing EET even in simple plasmonic antenna systems. These findings provide a real-time, quantum-mechanical perspective for understanding EET mechanisms and provide guidance in enhancing plasmonic properties in artificial light-harvesting systems.
Fil: Ilawe, Niranjan V.. University of California; Estados Unidos
Fil: Oviedo, María Belén. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Investigaciones en Físico-química de Córdoba. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Instituto de Investigaciones en Físico-química de Córdoba; Argentina. University of California; Estados Unidos
Fil: Wong, Bryan M.. University of California; Estados Unidos
Materia
Rt-Dftb
Energy Transfer
Nanoparticles
Plasmon
Nivel de accesibilidad
acceso abierto
Condiciones de uso
Atribución-NoComercial-CompartirIgual 2.5 Argentina (CC 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:11336/63868

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spelling Real-time quantum dynamics of long-range electronic excitation transfer in plasmonic nanoantennasIlawe, Niranjan V.Oviedo, María BelénWong, Bryan M.Rt-DftbEnergy TransferNanoparticlesPlasmonhttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1Using large-scale, real-time, quantum dynamics calculations, we present a detailed analysis of electronic excitation transfer (EET) mechanisms in a multiparticle plasmonic nanoantenna system. Specifically, we utilize real-time, time-dependent, density functional tight binding (RT-TDDFTB) to provide a quantum-mechanical description (at an electronic/atomistic level of detail) for characterizing and analyzing these systems, without recourse to classical approximations. We also demonstrate highly long-range electronic couplings in these complex systems and find that the range of these couplings is more than twice the conventional cutoff limit considered by Förster resonance energy transfer (FRET)-based approaches. Furthermore, we attribute these unusually long-ranged electronic couplings to the coherent oscillations of conduction electrons in plasmonic nanoparticles. This long-range nature of plasmonic interactions has important ramifications for EET; in particular, we show that the commonly used "nearest-neighbor" FRET model is inadequate for accurately characterizing EET even in simple plasmonic antenna systems. These findings provide a real-time, quantum-mechanical perspective for understanding EET mechanisms and provide guidance in enhancing plasmonic properties in artificial light-harvesting systems.Fil: Ilawe, Niranjan V.. University of California; Estados UnidosFil: Oviedo, María Belén. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Investigaciones en Físico-química de Córdoba. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Instituto de Investigaciones en Físico-química de Córdoba; Argentina. University of California; Estados UnidosFil: Wong, Bryan M.. University of California; Estados UnidosAmerican Chemical Society2017-08-05info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/63868Ilawe, Niranjan V.; Oviedo, María Belén; Wong, Bryan M.; Real-time quantum dynamics of long-range electronic excitation transfer in plasmonic nanoantennas; American Chemical Society; Journal of Chemical Theory and Computation; 13; 8; 5-8-2017; 3442-34541549-96181549-9626CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/http://pubs.acs.org/doi/abs/10.1021/acs.jctc.7b00423info:eu-repo/semantics/altIdentifier/doi/10.1021/acs.jctc.7b00423info:eu-repo/semantics/openAccessAtribución-NoComercial-CompartirIgual 2.5 Argentina (CC BY-NC-SA 2.5 AR)https://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-29T09:37:05Zoai:ri.conicet.gov.ar:11336/63868instacron: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 09:37:05.772CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Real-time quantum dynamics of long-range electronic excitation transfer in plasmonic nanoantennas
title Real-time quantum dynamics of long-range electronic excitation transfer in plasmonic nanoantennas
spellingShingle Real-time quantum dynamics of long-range electronic excitation transfer in plasmonic nanoantennas
Ilawe, Niranjan V.
Rt-Dftb
Energy Transfer
Nanoparticles
Plasmon
title_short Real-time quantum dynamics of long-range electronic excitation transfer in plasmonic nanoantennas
title_full Real-time quantum dynamics of long-range electronic excitation transfer in plasmonic nanoantennas
title_fullStr Real-time quantum dynamics of long-range electronic excitation transfer in plasmonic nanoantennas
title_full_unstemmed Real-time quantum dynamics of long-range electronic excitation transfer in plasmonic nanoantennas
title_sort Real-time quantum dynamics of long-range electronic excitation transfer in plasmonic nanoantennas
dc.creator.none.fl_str_mv Ilawe, Niranjan V.
Oviedo, María Belén
Wong, Bryan M.
author Ilawe, Niranjan V.
author_facet Ilawe, Niranjan V.
Oviedo, María Belén
Wong, Bryan M.
author_role author
author2 Oviedo, María Belén
Wong, Bryan M.
author2_role author
author
dc.subject.none.fl_str_mv Rt-Dftb
Energy Transfer
Nanoparticles
Plasmon
topic Rt-Dftb
Energy Transfer
Nanoparticles
Plasmon
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv Using large-scale, real-time, quantum dynamics calculations, we present a detailed analysis of electronic excitation transfer (EET) mechanisms in a multiparticle plasmonic nanoantenna system. Specifically, we utilize real-time, time-dependent, density functional tight binding (RT-TDDFTB) to provide a quantum-mechanical description (at an electronic/atomistic level of detail) for characterizing and analyzing these systems, without recourse to classical approximations. We also demonstrate highly long-range electronic couplings in these complex systems and find that the range of these couplings is more than twice the conventional cutoff limit considered by Förster resonance energy transfer (FRET)-based approaches. Furthermore, we attribute these unusually long-ranged electronic couplings to the coherent oscillations of conduction electrons in plasmonic nanoparticles. This long-range nature of plasmonic interactions has important ramifications for EET; in particular, we show that the commonly used "nearest-neighbor" FRET model is inadequate for accurately characterizing EET even in simple plasmonic antenna systems. These findings provide a real-time, quantum-mechanical perspective for understanding EET mechanisms and provide guidance in enhancing plasmonic properties in artificial light-harvesting systems.
Fil: Ilawe, Niranjan V.. University of California; Estados Unidos
Fil: Oviedo, María Belén. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Investigaciones en Físico-química de Córdoba. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Instituto de Investigaciones en Físico-química de Córdoba; Argentina. University of California; Estados Unidos
Fil: Wong, Bryan M.. University of California; Estados Unidos
description Using large-scale, real-time, quantum dynamics calculations, we present a detailed analysis of electronic excitation transfer (EET) mechanisms in a multiparticle plasmonic nanoantenna system. Specifically, we utilize real-time, time-dependent, density functional tight binding (RT-TDDFTB) to provide a quantum-mechanical description (at an electronic/atomistic level of detail) for characterizing and analyzing these systems, without recourse to classical approximations. We also demonstrate highly long-range electronic couplings in these complex systems and find that the range of these couplings is more than twice the conventional cutoff limit considered by Förster resonance energy transfer (FRET)-based approaches. Furthermore, we attribute these unusually long-ranged electronic couplings to the coherent oscillations of conduction electrons in plasmonic nanoparticles. This long-range nature of plasmonic interactions has important ramifications for EET; in particular, we show that the commonly used "nearest-neighbor" FRET model is inadequate for accurately characterizing EET even in simple plasmonic antenna systems. These findings provide a real-time, quantum-mechanical perspective for understanding EET mechanisms and provide guidance in enhancing plasmonic properties in artificial light-harvesting systems.
publishDate 2017
dc.date.none.fl_str_mv 2017-08-05
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/11336/63868
Ilawe, Niranjan V.; Oviedo, María Belén; Wong, Bryan M.; Real-time quantum dynamics of long-range electronic excitation transfer in plasmonic nanoantennas; American Chemical Society; Journal of Chemical Theory and Computation; 13; 8; 5-8-2017; 3442-3454
1549-9618
1549-9626
CONICET Digital
CONICET
url http://hdl.handle.net/11336/63868
identifier_str_mv Ilawe, Niranjan V.; Oviedo, María Belén; Wong, Bryan M.; Real-time quantum dynamics of long-range electronic excitation transfer in plasmonic nanoantennas; American Chemical Society; Journal of Chemical Theory and Computation; 13; 8; 5-8-2017; 3442-3454
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/http://pubs.acs.org/doi/abs/10.1021/acs.jctc.7b00423
info:eu-repo/semantics/altIdentifier/doi/10.1021/acs.jctc.7b00423
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
Atribución-NoComercial-CompartirIgual 2.5 Argentina (CC BY-NC-SA 2.5 AR)
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
eu_rights_str_mv openAccess
rights_invalid_str_mv Atribución-NoComercial-CompartirIgual 2.5 Argentina (CC BY-NC-SA 2.5 AR)
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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