Polymorphism and metal-induced structural transformation in 5,5′-bis(4-pyridyl)(2,2′-bispyrimidine) adlayers on Au(111)

Autores
Hötger, Diana; Carro, Pilar; Gutzler, Rico; Wurster, Benjamin; Chandrasekar, Rajadurai; Klyatskaya, Svetlana; Ruben, Mario; Salvarezza, Roberto Carlos; Kern, Klaus; Grumelli, Doris Elda
Año de publicación
2018
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
Metal-organic coordination networks self-assembled on surfaces have emerged as functional low-dimensional architectures with potential applications ranging from the fabrication of functional nanodevices to electrocatalysis. Among them, bis-pyridyl-bispyrimidine (PBP) and Fe-PBP on noble metal surfaces appear as interesting systems to reveal details of molecular self-assembly and the effect of metal incorporation on the organic network arrangement. Here, we report a combined STM, XPS, and DFT study revealing polymorphism for bis-pyridyl-bispyrimidine adsorbed adlayers on the reconstructed Au(111) surface. The polymorphic structures are converted by the addition of Fe adatoms into one unique Fe-PBP surface structure. DFT calculations show that while all PBP phases exhibit similar thermodynamic stability, metal incorporation selects the PBP structure which maximizes the number of Fe-N close contacts. Charge transfer from the Fe adatom to the Au substrate and N-Fe interactions stabilize the Fe-PBP adlayer. The increased thermodynamic stability of the metal-stabilized structure leads to its sole expression on the surface.
Fil: Hötger, Diana. Max Planck Institute for Solid State Research; Alemania
Fil: Carro, Pilar. Universidad de La Laguna; España
Fil: Gutzler, Rico. Max Planck Institute For Solid State Research; Alemania
Fil: Wurster, Benjamin. Max Planck Institute For Solid State Research; Alemania
Fil: Chandrasekar, Rajadurai. Karlsruher Institut fur Technologie; Alemania
Fil: Klyatskaya, Svetlana. Karlsruher Institut fur Technologie; Alemania
Fil: Ruben, Mario. Karlsruher Institut fur Technologie; Alemania. Université de Strasbourg; Francia
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
Fil: Kern, Klaus. Max Planck Institute For Solid State Research; Alemania. École Polytechnique Fédérale de Lausanne; Suiza
Fil: Grumelli, Doris Elda. 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
SELF ASSEMLED
2D METAL ORGANIC NETWORKS
STM DFT
XPS
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:11336/113511
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/113511
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repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Polymorphism and metal-induced structural transformation in 5,5′-bis(4-pyridyl)(2,2′-bispyrimidine) adlayers on Au(111)Hötger, DianaCarro, PilarGutzler, RicoWurster, BenjaminChandrasekar, RajaduraiKlyatskaya, SvetlanaRuben, MarioSalvarezza, Roberto CarlosKern, KlausGrumelli, Doris EldaSELF ASSEMLED2D METAL ORGANIC NETWORKSSTM DFTXPShttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1Metal-organic coordination networks self-assembled on surfaces have emerged as functional low-dimensional architectures with potential applications ranging from the fabrication of functional nanodevices to electrocatalysis. Among them, bis-pyridyl-bispyrimidine (PBP) and Fe-PBP on noble metal surfaces appear as interesting systems to reveal details of molecular self-assembly and the effect of metal incorporation on the organic network arrangement. Here, we report a combined STM, XPS, and DFT study revealing polymorphism for bis-pyridyl-bispyrimidine adsorbed adlayers on the reconstructed Au(111) surface. The polymorphic structures are converted by the addition of Fe adatoms into one unique Fe-PBP surface structure. DFT calculations show that while all PBP phases exhibit similar thermodynamic stability, metal incorporation selects the PBP structure which maximizes the number of Fe-N close contacts. Charge transfer from the Fe adatom to the Au substrate and N-Fe interactions stabilize the Fe-PBP adlayer. The increased thermodynamic stability of the metal-stabilized structure leads to its sole expression on the surface.Fil: Hötger, Diana. Max Planck Institute for Solid State Research; AlemaniaFil: Carro, Pilar. Universidad de La Laguna; EspañaFil: Gutzler, Rico. Max Planck Institute For Solid State Research; AlemaniaFil: Wurster, Benjamin. Max Planck Institute For Solid State Research; AlemaniaFil: Chandrasekar, Rajadurai. Karlsruher Institut fur Technologie; AlemaniaFil: Klyatskaya, Svetlana. Karlsruher Institut fur Technologie; AlemaniaFil: Ruben, Mario. Karlsruher Institut fur Technologie; Alemania. Université de Strasbourg; FranciaFil: 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; ArgentinaFil: Kern, Klaus. Max Planck Institute For Solid State Research; Alemania. École Polytechnique Fédérale de Lausanne; SuizaFil: Grumelli, Doris Elda. 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; ArgentinaRoyal Society of Chemistry2018-05info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/113511Hötger, Diana; Carro, Pilar; Gutzler, Rico; Wurster, Benjamin; Chandrasekar, Rajadurai; et al.; Polymorphism and metal-induced structural transformation in 5,5′-bis(4-pyridyl)(2,2′-bispyrimidine) adlayers on Au(111); Royal Society of Chemistry; Physical Chemistry Chemical Physics; 20; 23; 5-2018; 15960-159691463-9076CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/http://xlink.rsc.org/?DOI=C7CP07746Ginfo:eu-repo/semantics/altIdentifier/doi/10.1039/C7CP07746Ginfo:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-03T09:43:25Zoai:ri.conicet.gov.ar:11336/113511instacron: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:34982025-09-03 09:43:25.817CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Polymorphism and metal-induced structural transformation in 5,5′-bis(4-pyridyl)(2,2′-bispyrimidine) adlayers on Au(111)
title Polymorphism and metal-induced structural transformation in 5,5′-bis(4-pyridyl)(2,2′-bispyrimidine) adlayers on Au(111)
spellingShingle Polymorphism and metal-induced structural transformation in 5,5′-bis(4-pyridyl)(2,2′-bispyrimidine) adlayers on Au(111)
Hötger, Diana
SELF ASSEMLED
2D METAL ORGANIC NETWORKS
STM DFT
XPS
title_short Polymorphism and metal-induced structural transformation in 5,5′-bis(4-pyridyl)(2,2′-bispyrimidine) adlayers on Au(111)
title_full Polymorphism and metal-induced structural transformation in 5,5′-bis(4-pyridyl)(2,2′-bispyrimidine) adlayers on Au(111)
title_fullStr Polymorphism and metal-induced structural transformation in 5,5′-bis(4-pyridyl)(2,2′-bispyrimidine) adlayers on Au(111)
title_full_unstemmed Polymorphism and metal-induced structural transformation in 5,5′-bis(4-pyridyl)(2,2′-bispyrimidine) adlayers on Au(111)
title_sort Polymorphism and metal-induced structural transformation in 5,5′-bis(4-pyridyl)(2,2′-bispyrimidine) adlayers on Au(111)
dc.creator.none.fl_str_mv Hötger, Diana
Carro, Pilar
Gutzler, Rico
Wurster, Benjamin
Chandrasekar, Rajadurai
Klyatskaya, Svetlana
Ruben, Mario
Salvarezza, Roberto Carlos
Kern, Klaus
Grumelli, Doris Elda
author Hötger, Diana
author_facet Hötger, Diana
Carro, Pilar
Gutzler, Rico
Wurster, Benjamin
Chandrasekar, Rajadurai
Klyatskaya, Svetlana
Ruben, Mario
Salvarezza, Roberto Carlos
Kern, Klaus
Grumelli, Doris Elda
author_role author
author2 Carro, Pilar
Gutzler, Rico
Wurster, Benjamin
Chandrasekar, Rajadurai
Klyatskaya, Svetlana
Ruben, Mario
Salvarezza, Roberto Carlos
Kern, Klaus
Grumelli, Doris Elda
author2_role author
author
author
author
author
author
author
author
author
dc.subject.none.fl_str_mv SELF ASSEMLED
2D METAL ORGANIC NETWORKS
STM DFT
XPS
topic SELF ASSEMLED
2D METAL ORGANIC NETWORKS
STM DFT
XPS
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv Metal-organic coordination networks self-assembled on surfaces have emerged as functional low-dimensional architectures with potential applications ranging from the fabrication of functional nanodevices to electrocatalysis. Among them, bis-pyridyl-bispyrimidine (PBP) and Fe-PBP on noble metal surfaces appear as interesting systems to reveal details of molecular self-assembly and the effect of metal incorporation on the organic network arrangement. Here, we report a combined STM, XPS, and DFT study revealing polymorphism for bis-pyridyl-bispyrimidine adsorbed adlayers on the reconstructed Au(111) surface. The polymorphic structures are converted by the addition of Fe adatoms into one unique Fe-PBP surface structure. DFT calculations show that while all PBP phases exhibit similar thermodynamic stability, metal incorporation selects the PBP structure which maximizes the number of Fe-N close contacts. Charge transfer from the Fe adatom to the Au substrate and N-Fe interactions stabilize the Fe-PBP adlayer. The increased thermodynamic stability of the metal-stabilized structure leads to its sole expression on the surface.
Fil: Hötger, Diana. Max Planck Institute for Solid State Research; Alemania
Fil: Carro, Pilar. Universidad de La Laguna; España
Fil: Gutzler, Rico. Max Planck Institute For Solid State Research; Alemania
Fil: Wurster, Benjamin. Max Planck Institute For Solid State Research; Alemania
Fil: Chandrasekar, Rajadurai. Karlsruher Institut fur Technologie; Alemania
Fil: Klyatskaya, Svetlana. Karlsruher Institut fur Technologie; Alemania
Fil: Ruben, Mario. Karlsruher Institut fur Technologie; Alemania. Université de Strasbourg; Francia
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
Fil: Kern, Klaus. Max Planck Institute For Solid State Research; Alemania. École Polytechnique Fédérale de Lausanne; Suiza
Fil: Grumelli, Doris Elda. 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 Metal-organic coordination networks self-assembled on surfaces have emerged as functional low-dimensional architectures with potential applications ranging from the fabrication of functional nanodevices to electrocatalysis. Among them, bis-pyridyl-bispyrimidine (PBP) and Fe-PBP on noble metal surfaces appear as interesting systems to reveal details of molecular self-assembly and the effect of metal incorporation on the organic network arrangement. Here, we report a combined STM, XPS, and DFT study revealing polymorphism for bis-pyridyl-bispyrimidine adsorbed adlayers on the reconstructed Au(111) surface. The polymorphic structures are converted by the addition of Fe adatoms into one unique Fe-PBP surface structure. DFT calculations show that while all PBP phases exhibit similar thermodynamic stability, metal incorporation selects the PBP structure which maximizes the number of Fe-N close contacts. Charge transfer from the Fe adatom to the Au substrate and N-Fe interactions stabilize the Fe-PBP adlayer. The increased thermodynamic stability of the metal-stabilized structure leads to its sole expression on the surface.
publishDate 2018
dc.date.none.fl_str_mv 2018-05
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/11336/113511
Hötger, Diana; Carro, Pilar; Gutzler, Rico; Wurster, Benjamin; Chandrasekar, Rajadurai; et al.; Polymorphism and metal-induced structural transformation in 5,5′-bis(4-pyridyl)(2,2′-bispyrimidine) adlayers on Au(111); Royal Society of Chemistry; Physical Chemistry Chemical Physics; 20; 23; 5-2018; 15960-15969
1463-9076
CONICET Digital
CONICET
url http://hdl.handle.net/11336/113511
identifier_str_mv Hötger, Diana; Carro, Pilar; Gutzler, Rico; Wurster, Benjamin; Chandrasekar, Rajadurai; et al.; Polymorphism and metal-induced structural transformation in 5,5′-bis(4-pyridyl)(2,2′-bispyrimidine) adlayers on Au(111); Royal Society of Chemistry; Physical Chemistry Chemical Physics; 20; 23; 5-2018; 15960-15969
1463-9076
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://xlink.rsc.org/?DOI=C7CP07746G
info:eu-repo/semantics/altIdentifier/doi/10.1039/C7CP07746G
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
application/pdf
dc.publisher.none.fl_str_mv Royal Society of Chemistry
publisher.none.fl_str_mv Royal Society of Chemistry
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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score 13.13397

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