Why DFT-Based Tight Binding Gives a Better Representation of the Potential at Metal-Solution Interfaces than DFT Does

In modelling electrochemical interfaces it is important to treat electrode and electrolyte at the same level of theory. Density functional theory, which is usually the method of choice, suffers from a distinct disadvantage: The inner potential is calculated as the average of the total electrostatic...

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Autores: Quaino, Paola Monica, Nuñez, José Luis, Aradi, Bálint, van der Heide, Tammo, Santos, Elizabeth, Schmickler, Wolfgang
Formato: artículo
Estado:Versión publicada
Fecha de publicación:2023
País:Argentina
Recursos:Consejo Nacional de Investigaciones Científicas y Técnicas
Repositorio:CONICET Digital (CONICET)
Idioma:inglés
OAI Identifier:oai:ri.conicet.gov.ar:11336/226244
Acesso em linha:http://hdl.handle.net/11336/226244
Access Level:acceso abierto
Palavra-chave:DFT
INNER POTENTIAL
POTENTIAL OF ZERO CHARGE
TIGHT BINDING
WORK FUNCTION
https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
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spelling Why DFT-Based Tight Binding Gives a Better Representation of the Potential at Metal-Solution Interfaces than DFT DoesQuaino, Paola MonicaNuñez, José LuisAradi, Bálintvan der Heide, TammoSantos, ElizabethSchmickler, WolfgangDFTINNER POTENTIALPOTENTIAL OF ZERO CHARGETIGHT BINDINGWORK FUNCTIONhttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1In modelling electrochemical interfaces it is important to treat electrode and electrolyte at the same level of theory. Density functional theory, which is usually the method of choice, suffers from a distinct disadvantage: The inner potential is calculated as the average of the total electrostatic potential. This includes the highly localized potential generated from the nuclei. The resulting inner potential is far too high, of the order of 3.5 V, and not relevant for electrochemistry. In the density functional based tight binding (DFTB) method the electrostatic potential is much smoother, as it stems from atomic charge fluctuations with respect to neutral reference atoms. The resulting values for the electrochemical inner potential are much lower and compare well with those obtained by other, elaborate methods. Thus DFTB recommends itself as a method for treating the electrochemical interface including the inner potential.Fil: Quaino, Paola Monica. Universidad Nacional del Litoral. Instituto de Química Aplicada del Litoral. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Química Aplicada del Litoral.; ArgentinaFil: Nuñez, José Luis. Universidad Nacional del Litoral. Instituto de Química Aplicada del Litoral. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Química Aplicada del Litoral.; ArgentinaFil: Aradi, Bálint. Universitat Bremen; AlemaniaFil: van der Heide, Tammo. Universitat Bremen; AlemaniaFil: Santos, Elizabeth. Universitat Ulm; AlemaniaFil: Schmickler, Wolfgang. Universitat Ulm; AlemaniaJohn Wiley & Sons2023-10info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/226244Quaino, Paola Monica; Nuñez, José Luis; Aradi, Bálint; van der Heide, Tammo; Santos, Elizabeth; et al.; Why DFT-Based Tight Binding Gives a Better Representation of the Potential at Metal-Solution Interfaces than DFT Does; John Wiley & Sons; ChemElectroChem; 10; 20; 10-2023; 1-72196-0216CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/doi/10.1002/celc.202300230info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2024-05-08T14:22:33Zoai:ri.conicet.gov.ar:11336/226244instacron: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:34982024-05-08 14:22:33.32CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Why DFT-Based Tight Binding Gives a Better Representation of the Potential at Metal-Solution Interfaces than DFT Does
title Why DFT-Based Tight Binding Gives a Better Representation of the Potential at Metal-Solution Interfaces than DFT Does
spellingShingle Why DFT-Based Tight Binding Gives a Better Representation of the Potential at Metal-Solution Interfaces than DFT Does
Quaino, Paola Monica
DFT
INNER POTENTIAL
POTENTIAL OF ZERO CHARGE
TIGHT BINDING
WORK FUNCTION
https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
title_short Why DFT-Based Tight Binding Gives a Better Representation of the Potential at Metal-Solution Interfaces than DFT Does
title_full Why DFT-Based Tight Binding Gives a Better Representation of the Potential at Metal-Solution Interfaces than DFT Does
title_fullStr Why DFT-Based Tight Binding Gives a Better Representation of the Potential at Metal-Solution Interfaces than DFT Does
title_full_unstemmed Why DFT-Based Tight Binding Gives a Better Representation of the Potential at Metal-Solution Interfaces than DFT Does
title_sort Why DFT-Based Tight Binding Gives a Better Representation of the Potential at Metal-Solution Interfaces than DFT Does
dc.creator.none.fl_str_mv Quaino, Paola Monica
Nuñez, José Luis
Aradi, Bálint
van der Heide, Tammo
Santos, Elizabeth
Schmickler, Wolfgang
author Quaino, Paola Monica
author_facet Quaino, Paola Monica
Nuñez, José Luis
Aradi, Bálint
van der Heide, Tammo
Santos, Elizabeth
Schmickler, Wolfgang
author_role author
author2 Nuñez, José Luis
Aradi, Bálint
van der Heide, Tammo
Santos, Elizabeth
Schmickler, Wolfgang
author2_role author
author
author
author
author
dc.subject.none.fl_str_mv DFT
INNER POTENTIAL
POTENTIAL OF ZERO CHARGE
TIGHT BINDING
WORK FUNCTION
https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
topic DFT
INNER POTENTIAL
POTENTIAL OF ZERO CHARGE
TIGHT BINDING
WORK FUNCTION
https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
description In modelling electrochemical interfaces it is important to treat electrode and electrolyte at the same level of theory. Density functional theory, which is usually the method of choice, suffers from a distinct disadvantage: The inner potential is calculated as the average of the total electrostatic potential. This includes the highly localized potential generated from the nuclei. The resulting inner potential is far too high, of the order of 3.5 V, and not relevant for electrochemistry. In the density functional based tight binding (DFTB) method the electrostatic potential is much smoother, as it stems from atomic charge fluctuations with respect to neutral reference atoms. The resulting values for the electrochemical inner potential are much lower and compare well with those obtained by other, elaborate methods. Thus DFTB recommends itself as a method for treating the electrochemical interface including the inner potential.
publishDate 2023
dc.date.none.fl_str_mv 2023-10
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/11336/226244
Quaino, Paola Monica; Nuñez, José Luis; Aradi, Bálint; van der Heide, Tammo; Santos, Elizabeth; et al.; Why DFT-Based Tight Binding Gives a Better Representation of the Potential at Metal-Solution Interfaces than DFT Does; John Wiley & Sons; ChemElectroChem; 10; 20; 10-2023; 1-7
2196-0216
CONICET Digital
CONICET
url http://hdl.handle.net/11336/226244
identifier_str_mv Quaino, Paola Monica; Nuñez, José Luis; Aradi, Bálint; van der Heide, Tammo; Santos, Elizabeth; et al.; Why DFT-Based Tight Binding Gives a Better Representation of the Potential at Metal-Solution Interfaces than DFT Does; John Wiley & Sons; ChemElectroChem; 10; 20; 10-2023; 1-7
2196-0216
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/doi/10.1002/celc.202300230
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
https://creativecommons.org/licenses/by/2.5/ar/
eu_rights_str_mv openAccess
rights_invalid_str_mv https://creativecommons.org/licenses/by/2.5/ar/
dc.format.none.fl_str_mv application/pdf
application/pdf
dc.publisher.none.fl_str_mv John Wiley & Sons
publisher.none.fl_str_mv John Wiley & Sons
dc.source.none.fl_str_mv reponame:CONICET Digital (CONICET)
instname:Consejo Nacional de Investigaciones Científicas y Técnicas
instname_str Consejo Nacional de Investigaciones Científicas y Técnicas
reponame_str CONICET Digital (CONICET)
collection CONICET Digital (CONICET)
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 15.812429

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