Molecular dissociation in the presence of catalysts: Interpreting bond breaking as a quantum dynamical phase transition

Autores
Ruderman, Andres; Dente, Axel Damián; Santos, Elizabeth del Carmen; Pastawski, Horacio Miguel
Año de publicación
2015
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
In this work we show that molecular chemical bond formation and dissociation in the presence of the d-band of a metal catalyst can be described as a quantum dynamical phase transition (QDPT). This agrees with DFT calculations that predict sudden jumps in some observables as the molecule breaks. According to our model this phenomenon emerges because the catalyst provides for a non-Hermitian Hamiltonian. We show that when the molecule approaches the surface, as occurs in the Heyrovsky reaction of H2, the bonding H2 orbital has a smooth crossover into a bonding molecular orbital built with the closest H orbital and the surface metal d-states. The same occurs for the antibonding state. Meanwhile, two resonances appear within the continuous spectrum of the d-band, which are associated with bonding and antibonding orbitals between the furthest H atom and the d-states at the second metallic layer. These move toward the band center, where they collapse into a pure metallic resonance and an almost isolated H orbital. This phenomenon constitutes a striking example of the non-trivial physics enabled when one deals with non-Hermitian Hamiltonian beyond the usual wide band approximation.
Fil: Ruderman, Andres. Universitat Ulm; Alemania. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Física Enrique Gaviola. Universidad Nacional de Córdoba. Instituto de Física Enrique Gaviola; Argentina
Fil: Dente, Axel Damián. Invap S. E.; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Fil: Santos, Elizabeth del Carmen. Universitat Ulm; Alemania. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Física Enrique Gaviola. Universidad Nacional de Córdoba. Instituto de Física Enrique Gaviola; Argentina
Fil: Pastawski, Horacio Miguel. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Física Enrique Gaviola. Universidad Nacional de Córdoba. Instituto de Física Enrique Gaviola; Argentina
Materia
ATOMS
MOLECULE
TRANSITION
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:11336/185734
Acceder
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spelling Molecular dissociation in the presence of catalysts: Interpreting bond breaking as a quantum dynamical phase transitionRuderman, AndresDente, Axel DamiánSantos, Elizabeth del CarmenPastawski, Horacio MiguelATOMSMOLECULETRANSITIONhttps://purl.org/becyt/ford/1.3https://purl.org/becyt/ford/1In this work we show that molecular chemical bond formation and dissociation in the presence of the d-band of a metal catalyst can be described as a quantum dynamical phase transition (QDPT). This agrees with DFT calculations that predict sudden jumps in some observables as the molecule breaks. According to our model this phenomenon emerges because the catalyst provides for a non-Hermitian Hamiltonian. We show that when the molecule approaches the surface, as occurs in the Heyrovsky reaction of H2, the bonding H2 orbital has a smooth crossover into a bonding molecular orbital built with the closest H orbital and the surface metal d-states. The same occurs for the antibonding state. Meanwhile, two resonances appear within the continuous spectrum of the d-band, which are associated with bonding and antibonding orbitals between the furthest H atom and the d-states at the second metallic layer. These move toward the band center, where they collapse into a pure metallic resonance and an almost isolated H orbital. This phenomenon constitutes a striking example of the non-trivial physics enabled when one deals with non-Hermitian Hamiltonian beyond the usual wide band approximation.Fil: Ruderman, Andres. Universitat Ulm; Alemania. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Física Enrique Gaviola. Universidad Nacional de Córdoba. Instituto de Física Enrique Gaviola; ArgentinaFil: Dente, Axel Damián. Invap S. E.; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; ArgentinaFil: Santos, Elizabeth del Carmen. Universitat Ulm; Alemania. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Física Enrique Gaviola. Universidad Nacional de Córdoba. Instituto de Física Enrique Gaviola; ArgentinaFil: Pastawski, Horacio Miguel. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Física Enrique Gaviola. Universidad Nacional de Córdoba. Instituto de Física Enrique Gaviola; ArgentinaIOP Publishing2015-08info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/185734Ruderman, Andres; Dente, Axel Damián; Santos, Elizabeth del Carmen; Pastawski, Horacio Miguel; Molecular dissociation in the presence of catalysts: Interpreting bond breaking as a quantum dynamical phase transition; IOP Publishing; Journal of Physics: Condensed Matter; 27; 31; 8-2015; 1-70953-89841361-648XCONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/https://iopscience.iop.org/article/10.1088/0953-8984/27/31/315501info:eu-repo/semantics/altIdentifier/doi/10.1088/0953-8984/27/31/315501info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-29T09:40:55Zoai:ri.conicet.gov.ar:11336/185734instacron: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 09:40:55.455CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Molecular dissociation in the presence of catalysts: Interpreting bond breaking as a quantum dynamical phase transition
title Molecular dissociation in the presence of catalysts: Interpreting bond breaking as a quantum dynamical phase transition
spellingShingle Molecular dissociation in the presence of catalysts: Interpreting bond breaking as a quantum dynamical phase transition
Ruderman, Andres
ATOMS
MOLECULE
TRANSITION
title_short Molecular dissociation in the presence of catalysts: Interpreting bond breaking as a quantum dynamical phase transition
title_full Molecular dissociation in the presence of catalysts: Interpreting bond breaking as a quantum dynamical phase transition
title_fullStr Molecular dissociation in the presence of catalysts: Interpreting bond breaking as a quantum dynamical phase transition
title_full_unstemmed Molecular dissociation in the presence of catalysts: Interpreting bond breaking as a quantum dynamical phase transition
title_sort Molecular dissociation in the presence of catalysts: Interpreting bond breaking as a quantum dynamical phase transition
dc.creator.none.fl_str_mv Ruderman, Andres
Dente, Axel Damián
Santos, Elizabeth del Carmen
Pastawski, Horacio Miguel
author Ruderman, Andres
author_facet Ruderman, Andres
Dente, Axel Damián
Santos, Elizabeth del Carmen
Pastawski, Horacio Miguel
author_role author
author2 Dente, Axel Damián
Santos, Elizabeth del Carmen
Pastawski, Horacio Miguel
author2_role author
author
author
dc.subject.none.fl_str_mv ATOMS
MOLECULE
TRANSITION
topic ATOMS
MOLECULE
TRANSITION
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.3
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv In this work we show that molecular chemical bond formation and dissociation in the presence of the d-band of a metal catalyst can be described as a quantum dynamical phase transition (QDPT). This agrees with DFT calculations that predict sudden jumps in some observables as the molecule breaks. According to our model this phenomenon emerges because the catalyst provides for a non-Hermitian Hamiltonian. We show that when the molecule approaches the surface, as occurs in the Heyrovsky reaction of H2, the bonding H2 orbital has a smooth crossover into a bonding molecular orbital built with the closest H orbital and the surface metal d-states. The same occurs for the antibonding state. Meanwhile, two resonances appear within the continuous spectrum of the d-band, which are associated with bonding and antibonding orbitals between the furthest H atom and the d-states at the second metallic layer. These move toward the band center, where they collapse into a pure metallic resonance and an almost isolated H orbital. This phenomenon constitutes a striking example of the non-trivial physics enabled when one deals with non-Hermitian Hamiltonian beyond the usual wide band approximation.
Fil: Ruderman, Andres. Universitat Ulm; Alemania. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Física Enrique Gaviola. Universidad Nacional de Córdoba. Instituto de Física Enrique Gaviola; Argentina
Fil: Dente, Axel Damián. Invap S. E.; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Fil: Santos, Elizabeth del Carmen. Universitat Ulm; Alemania. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Física Enrique Gaviola. Universidad Nacional de Córdoba. Instituto de Física Enrique Gaviola; Argentina
Fil: Pastawski, Horacio Miguel. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Física Enrique Gaviola. Universidad Nacional de Córdoba. Instituto de Física Enrique Gaviola; Argentina
description In this work we show that molecular chemical bond formation and dissociation in the presence of the d-band of a metal catalyst can be described as a quantum dynamical phase transition (QDPT). This agrees with DFT calculations that predict sudden jumps in some observables as the molecule breaks. According to our model this phenomenon emerges because the catalyst provides for a non-Hermitian Hamiltonian. We show that when the molecule approaches the surface, as occurs in the Heyrovsky reaction of H2, the bonding H2 orbital has a smooth crossover into a bonding molecular orbital built with the closest H orbital and the surface metal d-states. The same occurs for the antibonding state. Meanwhile, two resonances appear within the continuous spectrum of the d-band, which are associated with bonding and antibonding orbitals between the furthest H atom and the d-states at the second metallic layer. These move toward the band center, where they collapse into a pure metallic resonance and an almost isolated H orbital. This phenomenon constitutes a striking example of the non-trivial physics enabled when one deals with non-Hermitian Hamiltonian beyond the usual wide band approximation.
publishDate 2015
dc.date.none.fl_str_mv 2015-08
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/11336/185734
Ruderman, Andres; Dente, Axel Damián; Santos, Elizabeth del Carmen; Pastawski, Horacio Miguel; Molecular dissociation in the presence of catalysts: Interpreting bond breaking as a quantum dynamical phase transition; IOP Publishing; Journal of Physics: Condensed Matter; 27; 31; 8-2015; 1-7
0953-8984
1361-648X
CONICET Digital
CONICET
url http://hdl.handle.net/11336/185734
identifier_str_mv Ruderman, Andres; Dente, Axel Damián; Santos, Elizabeth del Carmen; Pastawski, Horacio Miguel; Molecular dissociation in the presence of catalysts: Interpreting bond breaking as a quantum dynamical phase transition; IOP Publishing; Journal of Physics: Condensed Matter; 27; 31; 8-2015; 1-7
0953-8984
1361-648X
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://iopscience.iop.org/article/10.1088/0953-8984/27/31/315501
info:eu-repo/semantics/altIdentifier/doi/10.1088/0953-8984/27/31/315501
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 IOP Publishing
publisher.none.fl_str_mv IOP Publishing
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 13.070432

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