Bias-dependent local structure of water molecules at a metallic interface
Autor(a) principal: | |
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Data de Publicação: | 2018 |
Outros Autores: | , , |
Tipo de documento: | Artigo |
Idioma: | eng |
Título da fonte: | Repositório Institucional da UNESP |
Texto Completo: | http://dx.doi.org/10.1039/c7sc02208e http://hdl.handle.net/11449/163646 |
Resumo: | Understanding the local structure of water at the interfaces of metallic electrodes is a key issue in aqueousbased electrochemistry. Nevertheless a realistic simulation of such a setup is challenging, particularly when the electrodes are maintained at different potentials. To correctly compute the effect of an external bias potential applied to truly semi-infinite surfaces, we combine Density Functional Theory (DFT) and NonEquilibrium Green's Function (NEGF) methods. This framework allows for the out-of-equilibrium calculation of forces and dynamics, and directly correlates to the chemical potential of the electrodes, which is introduced experimentally. In this work, we apply this methodology to study the electronic properties and atomic forces of a water molecule at the interface of a gold surface. We find that the water molecule tends to align its dipole moment with the electric field, and it is either repelled or attracted to the metal depending on the sign and magnitude of the applied bias, in an asymmetric fashion. |
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Bias-dependent local structure of water molecules at a metallic interfaceUnderstanding the local structure of water at the interfaces of metallic electrodes is a key issue in aqueousbased electrochemistry. Nevertheless a realistic simulation of such a setup is challenging, particularly when the electrodes are maintained at different potentials. To correctly compute the effect of an external bias potential applied to truly semi-infinite surfaces, we combine Density Functional Theory (DFT) and NonEquilibrium Green's Function (NEGF) methods. This framework allows for the out-of-equilibrium calculation of forces and dynamics, and directly correlates to the chemical potential of the electrodes, which is introduced experimentally. In this work, we apply this methodology to study the electronic properties and atomic forces of a water molecule at the interface of a gold surface. We find that the water molecule tends to align its dipole moment with the electric field, and it is either repelled or attracted to the metal depending on the sign and magnitude of the applied bias, in an asymmetric fashion.DOE Early Career AwardsFundação de Amparo à Pesquisa do Estado de São Paulo (FAPESP)ICTP-Simons Associate SchemeFP7 FET-ICT Planar Atomic and Molecular Scale devices (PAMS) project (European Commission)Spanish Agencia Estatal de InvestigacionDep. de Educacion of the Basque GovernmentUPV/EHUUS Department of EnergyUniv Estadual Paulista, Inst Fis Teor, ICTP South Amer Inst Fundamental Res, BR-01140070 Sao Paulo, SP, BrazilUniv Fed ABC, Ctr Ciencias Nat & Humanas, BR-09210170 Santo Andre, SP, BrazilCtr Fis Mat, Donostia San Sebastian 20018, Gipuzkoa, SpainDonostia Int Phys Ctr, Donostia San Sebastian 20018, Gipuzkoa, SpainUniv Estadual Paulista, Inst Fis Teor, BR-01140070 Sao Paulo, SP, BrazilSUNY Stony Brook, Dept Phys & Astron, Stony Brook, NY 11794 USASUNY Stony Brook, Inst Adv Computat Sci, Stony Brook, NY 11794 USAUniv Estadual Paulista, Inst Fis Teor, ICTP South Amer Inst Fundamental Res, BR-01140070 Sao Paulo, SP, BrazilUniv Estadual Paulista, Inst Fis Teor, BR-01140070 Sao Paulo, SP, BrazilDOE Early Career Awards: DE-SC0003871DOE Early Career Awards: DE-FG02-09ER16052FAPESP: 2011/11973-4FP7 FET-ICT Planar Atomic and Molecular Scale devices (PAMS) project (European Commission): 610446Spanish Agencia Estatal de Investigacion: MAT2016-78293-C6-4-RUPV/EHU: IT-756-13US Department of Energy: DE-AC02-98CH10886Royal Soc ChemistryUniversidade Estadual Paulista (Unesp)Universidade Federal do ABC (UFABC)Ctr Fis MatDonostia Int Phys CtrSUNY Stony BrookPedroza, Luana S. [UNESP]Brandimarte, PedroRocha, Alexandre Reily [UNESP]Fernandez-Serra, M. -V.2018-11-26T17:44:24Z2018-11-26T17:44:24Z2018-01-07info:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/article62-69application/pdfhttp://dx.doi.org/10.1039/c7sc02208eChemical Science. Cambridge: Royal Soc Chemistry, v. 9, n. 1, p. 62-69, 2018.2041-6520http://hdl.handle.net/11449/16364610.1039/c7sc02208eWOS:000418376400007WOS000418376400007.pdfWeb of Sciencereponame:Repositório Institucional da UNESPinstname:Universidade Estadual Paulista (UNESP)instacron:UNESPengChemical Science4,508info:eu-repo/semantics/openAccess2023-12-18T06:19:11Zoai:repositorio.unesp.br:11449/163646Repositório InstitucionalPUBhttp://repositorio.unesp.br/oai/requestopendoar:29462024-08-05T20:40:59.157652Repositório Institucional da UNESP - Universidade Estadual Paulista (UNESP)false |
dc.title.none.fl_str_mv |
Bias-dependent local structure of water molecules at a metallic interface |
title |
Bias-dependent local structure of water molecules at a metallic interface |
spellingShingle |
Bias-dependent local structure of water molecules at a metallic interface Pedroza, Luana S. [UNESP] |
title_short |
Bias-dependent local structure of water molecules at a metallic interface |
title_full |
Bias-dependent local structure of water molecules at a metallic interface |
title_fullStr |
Bias-dependent local structure of water molecules at a metallic interface |
title_full_unstemmed |
Bias-dependent local structure of water molecules at a metallic interface |
title_sort |
Bias-dependent local structure of water molecules at a metallic interface |
author |
Pedroza, Luana S. [UNESP] |
author_facet |
Pedroza, Luana S. [UNESP] Brandimarte, Pedro Rocha, Alexandre Reily [UNESP] Fernandez-Serra, M. -V. |
author_role |
author |
author2 |
Brandimarte, Pedro Rocha, Alexandre Reily [UNESP] Fernandez-Serra, M. -V. |
author2_role |
author author author |
dc.contributor.none.fl_str_mv |
Universidade Estadual Paulista (Unesp) Universidade Federal do ABC (UFABC) Ctr Fis Mat Donostia Int Phys Ctr SUNY Stony Brook |
dc.contributor.author.fl_str_mv |
Pedroza, Luana S. [UNESP] Brandimarte, Pedro Rocha, Alexandre Reily [UNESP] Fernandez-Serra, M. -V. |
description |
Understanding the local structure of water at the interfaces of metallic electrodes is a key issue in aqueousbased electrochemistry. Nevertheless a realistic simulation of such a setup is challenging, particularly when the electrodes are maintained at different potentials. To correctly compute the effect of an external bias potential applied to truly semi-infinite surfaces, we combine Density Functional Theory (DFT) and NonEquilibrium Green's Function (NEGF) methods. This framework allows for the out-of-equilibrium calculation of forces and dynamics, and directly correlates to the chemical potential of the electrodes, which is introduced experimentally. In this work, we apply this methodology to study the electronic properties and atomic forces of a water molecule at the interface of a gold surface. We find that the water molecule tends to align its dipole moment with the electric field, and it is either repelled or attracted to the metal depending on the sign and magnitude of the applied bias, in an asymmetric fashion. |
publishDate |
2018 |
dc.date.none.fl_str_mv |
2018-11-26T17:44:24Z 2018-11-26T17:44:24Z 2018-01-07 |
dc.type.status.fl_str_mv |
info:eu-repo/semantics/publishedVersion |
dc.type.driver.fl_str_mv |
info:eu-repo/semantics/article |
format |
article |
status_str |
publishedVersion |
dc.identifier.uri.fl_str_mv |
http://dx.doi.org/10.1039/c7sc02208e Chemical Science. Cambridge: Royal Soc Chemistry, v. 9, n. 1, p. 62-69, 2018. 2041-6520 http://hdl.handle.net/11449/163646 10.1039/c7sc02208e WOS:000418376400007 WOS000418376400007.pdf |
url |
http://dx.doi.org/10.1039/c7sc02208e http://hdl.handle.net/11449/163646 |
identifier_str_mv |
Chemical Science. Cambridge: Royal Soc Chemistry, v. 9, n. 1, p. 62-69, 2018. 2041-6520 10.1039/c7sc02208e WOS:000418376400007 WOS000418376400007.pdf |
dc.language.iso.fl_str_mv |
eng |
language |
eng |
dc.relation.none.fl_str_mv |
Chemical Science 4,508 |
dc.rights.driver.fl_str_mv |
info:eu-repo/semantics/openAccess |
eu_rights_str_mv |
openAccess |
dc.format.none.fl_str_mv |
62-69 application/pdf |
dc.publisher.none.fl_str_mv |
Royal Soc Chemistry |
publisher.none.fl_str_mv |
Royal Soc Chemistry |
dc.source.none.fl_str_mv |
Web of Science reponame:Repositório Institucional da UNESP instname:Universidade Estadual Paulista (UNESP) instacron:UNESP |
instname_str |
Universidade Estadual Paulista (UNESP) |
instacron_str |
UNESP |
institution |
UNESP |
reponame_str |
Repositório Institucional da UNESP |
collection |
Repositório Institucional da UNESP |
repository.name.fl_str_mv |
Repositório Institucional da UNESP - Universidade Estadual Paulista (UNESP) |
repository.mail.fl_str_mv |
|
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1808129233704189952 |