On the Thermodynamic Stability of α,ω-Alkanedithiols Self-Assembled Monolayers on Unreconstructed and Reconstructed Au(111)

Autores
Carro, P.; Hernández Creus, A.; Muñoz, A.; Salvarezza, Roberto Carlos
Año de publicación
2010
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
A comparative study on the thermodynamic stability of the lying down (LD) and standing up (SU) phases of α,ω-butanedithiol (BDT) on unreconstructed (U) and on reconstructed (R) Au(111) surfaces is presented. The R surface is made of dithiol-Au adatom units. Density functional calculations (DFT) allow the estimation of the adsorption energy of the LD and SU BDT phases on both substrates. Surface free energies based on the DFT calculations show the coverage of the clean Au(111) surface by the LD phase, and the LD to SU phase transition as the chemical potential of the BDT molecule is increased. The LD and SU phases are more stable on R than on U substrates, suggesting that the Au(111) surface should reconstruct upon BDT adsorption. The stability analysis is extended to longer α,ω-dithiols. Results reveal that the LD to SU phase transition is favored as the hydrocarbon chain length of the dithiol molecule is increased. Changes in the hydrogen pressure affect the formation of the LD phase, while they have only minor effects on the LD to SU phase transitions. Our calculations explain the influence of the number of carbon atoms in the hydrocarbon chains, hydrogen pressure and dithiol pressure (or concentration) on dithiol adsorption, and phase transitions. This information is relevant to control the coverage, reactivity, and surface chemistry of the α,ω-dithiol self-assembled monolayers on Au surfaces.
Fil: Carro, P.. Universidad de La Laguna; España
Fil: Hernández Creus, A.. Universidad de La Laguna; España
Fil: Muñoz, A.. Universidad de La Laguna; España
Fil: Salvarezza, Roberto Carlos. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas. Universidad Nacional de La Plata. Facultad de Ciencias Exactas. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas; Argentina
Materia
Dithiols
Au(111)
DFT
Thermodynamics
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:11336/278335
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/278335
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling On the Thermodynamic Stability of α,ω-Alkanedithiols Self-Assembled Monolayers on Unreconstructed and Reconstructed Au(111)Carro, P.Hernández Creus, A.Muñoz, A.Salvarezza, Roberto CarlosDithiolsAu(111)DFTThermodynamicshttps://purl.org/becyt/ford/2.10https://purl.org/becyt/ford/2A comparative study on the thermodynamic stability of the lying down (LD) and standing up (SU) phases of α,ω-butanedithiol (BDT) on unreconstructed (U) and on reconstructed (R) Au(111) surfaces is presented. The R surface is made of dithiol-Au adatom units. Density functional calculations (DFT) allow the estimation of the adsorption energy of the LD and SU BDT phases on both substrates. Surface free energies based on the DFT calculations show the coverage of the clean Au(111) surface by the LD phase, and the LD to SU phase transition as the chemical potential of the BDT molecule is increased. The LD and SU phases are more stable on R than on U substrates, suggesting that the Au(111) surface should reconstruct upon BDT adsorption. The stability analysis is extended to longer α,ω-dithiols. Results reveal that the LD to SU phase transition is favored as the hydrocarbon chain length of the dithiol molecule is increased. Changes in the hydrogen pressure affect the formation of the LD phase, while they have only minor effects on the LD to SU phase transitions. Our calculations explain the influence of the number of carbon atoms in the hydrocarbon chains, hydrogen pressure and dithiol pressure (or concentration) on dithiol adsorption, and phase transitions. This information is relevant to control the coverage, reactivity, and surface chemistry of the α,ω-dithiol self-assembled monolayers on Au surfaces.Fil: Carro, P.. Universidad de La Laguna; EspañaFil: Hernández Creus, A.. Universidad de La Laguna; EspañaFil: Muñoz, A.. Universidad de La Laguna; EspañaFil: Salvarezza, Roberto Carlos. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas. Universidad Nacional de La Plata. Facultad de Ciencias Exactas. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas; ArgentinaAmerican Chemical Society2010-05info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/278335Carro, P.; Hernández Creus, A.; Muñoz, A.; Salvarezza, Roberto Carlos; On the Thermodynamic Stability of α,ω-Alkanedithiols Self-Assembled Monolayers on Unreconstructed and Reconstructed Au(111); American Chemical Society; Langmuir; 26; 12; 5-2010; 9589-95950743-7463CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/https://pubs.acs.org/doi/10.1021/la100167binfo:eu-repo/semantics/altIdentifier/doi/10.1021/la100167binfo:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2026-01-08T12:56:15Zoai:ri.conicet.gov.ar:11336/278335instacron: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:34982026-01-08 12:56:15.317CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv On the Thermodynamic Stability of α,ω-Alkanedithiols Self-Assembled Monolayers on Unreconstructed and Reconstructed Au(111)
title On the Thermodynamic Stability of α,ω-Alkanedithiols Self-Assembled Monolayers on Unreconstructed and Reconstructed Au(111)
spellingShingle On the Thermodynamic Stability of α,ω-Alkanedithiols Self-Assembled Monolayers on Unreconstructed and Reconstructed Au(111)
Carro, P.
Dithiols
Au(111)
DFT
Thermodynamics
title_short On the Thermodynamic Stability of α,ω-Alkanedithiols Self-Assembled Monolayers on Unreconstructed and Reconstructed Au(111)
title_full On the Thermodynamic Stability of α,ω-Alkanedithiols Self-Assembled Monolayers on Unreconstructed and Reconstructed Au(111)
title_fullStr On the Thermodynamic Stability of α,ω-Alkanedithiols Self-Assembled Monolayers on Unreconstructed and Reconstructed Au(111)
title_full_unstemmed On the Thermodynamic Stability of α,ω-Alkanedithiols Self-Assembled Monolayers on Unreconstructed and Reconstructed Au(111)
title_sort On the Thermodynamic Stability of α,ω-Alkanedithiols Self-Assembled Monolayers on Unreconstructed and Reconstructed Au(111)
dc.creator.none.fl_str_mv Carro, P.
Hernández Creus, A.
Muñoz, A.
Salvarezza, Roberto Carlos
author Carro, P.
author_facet Carro, P.
Hernández Creus, A.
Muñoz, A.
Salvarezza, Roberto Carlos
author_role author
author2 Hernández Creus, A.
Muñoz, A.
Salvarezza, Roberto Carlos
author2_role author
author
author
dc.subject.none.fl_str_mv Dithiols
Au(111)
DFT
Thermodynamics
topic Dithiols
Au(111)
DFT
Thermodynamics
purl_subject.fl_str_mv https://purl.org/becyt/ford/2.10
https://purl.org/becyt/ford/2
dc.description.none.fl_txt_mv A comparative study on the thermodynamic stability of the lying down (LD) and standing up (SU) phases of α,ω-butanedithiol (BDT) on unreconstructed (U) and on reconstructed (R) Au(111) surfaces is presented. The R surface is made of dithiol-Au adatom units. Density functional calculations (DFT) allow the estimation of the adsorption energy of the LD and SU BDT phases on both substrates. Surface free energies based on the DFT calculations show the coverage of the clean Au(111) surface by the LD phase, and the LD to SU phase transition as the chemical potential of the BDT molecule is increased. The LD and SU phases are more stable on R than on U substrates, suggesting that the Au(111) surface should reconstruct upon BDT adsorption. The stability analysis is extended to longer α,ω-dithiols. Results reveal that the LD to SU phase transition is favored as the hydrocarbon chain length of the dithiol molecule is increased. Changes in the hydrogen pressure affect the formation of the LD phase, while they have only minor effects on the LD to SU phase transitions. Our calculations explain the influence of the number of carbon atoms in the hydrocarbon chains, hydrogen pressure and dithiol pressure (or concentration) on dithiol adsorption, and phase transitions. This information is relevant to control the coverage, reactivity, and surface chemistry of the α,ω-dithiol self-assembled monolayers on Au surfaces.
Fil: Carro, P.. Universidad de La Laguna; España
Fil: Hernández Creus, A.. Universidad de La Laguna; España
Fil: Muñoz, A.. Universidad de La Laguna; España
Fil: Salvarezza, Roberto Carlos. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas. Universidad Nacional de La Plata. Facultad de Ciencias Exactas. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas; Argentina
description A comparative study on the thermodynamic stability of the lying down (LD) and standing up (SU) phases of α,ω-butanedithiol (BDT) on unreconstructed (U) and on reconstructed (R) Au(111) surfaces is presented. The R surface is made of dithiol-Au adatom units. Density functional calculations (DFT) allow the estimation of the adsorption energy of the LD and SU BDT phases on both substrates. Surface free energies based on the DFT calculations show the coverage of the clean Au(111) surface by the LD phase, and the LD to SU phase transition as the chemical potential of the BDT molecule is increased. The LD and SU phases are more stable on R than on U substrates, suggesting that the Au(111) surface should reconstruct upon BDT adsorption. The stability analysis is extended to longer α,ω-dithiols. Results reveal that the LD to SU phase transition is favored as the hydrocarbon chain length of the dithiol molecule is increased. Changes in the hydrogen pressure affect the formation of the LD phase, while they have only minor effects on the LD to SU phase transitions. Our calculations explain the influence of the number of carbon atoms in the hydrocarbon chains, hydrogen pressure and dithiol pressure (or concentration) on dithiol adsorption, and phase transitions. This information is relevant to control the coverage, reactivity, and surface chemistry of the α,ω-dithiol self-assembled monolayers on Au surfaces.
publishDate 2010
dc.date.none.fl_str_mv 2010-05
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/11336/278335
Carro, P.; Hernández Creus, A.; Muñoz, A.; Salvarezza, Roberto Carlos; On the Thermodynamic Stability of α,ω-Alkanedithiols Self-Assembled Monolayers on Unreconstructed and Reconstructed Au(111); American Chemical Society; Langmuir; 26; 12; 5-2010; 9589-9595
0743-7463
CONICET Digital
CONICET
url http://hdl.handle.net/11336/278335
identifier_str_mv Carro, P.; Hernández Creus, A.; Muñoz, A.; Salvarezza, Roberto Carlos; On the Thermodynamic Stability of α,ω-Alkanedithiols Self-Assembled Monolayers on Unreconstructed and Reconstructed Au(111); American Chemical Society; Langmuir; 26; 12; 5-2010; 9589-9595
0743-7463
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/la100167b
info:eu-repo/semantics/altIdentifier/doi/10.1021/la100167b
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
_version_ 1853775408417210368
score 13.25844

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