Rational Design of 2D Supramolecular Networks Switchable by External Electric Fields

Autores
Cometto, Fernando Pablo; Arisnabarreta, Nicolás; Vanta, Radovan; Jacquelin, Daniela Karina; Vyas, Vijay; Lotsch, Bettina V.; Paredes Olivera, Patricia; Patrito, Eduardo Martin; Lingenfelder, Magalí Alejandra
Año de publicación
2024
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
The reversible formation of hydrogen bonds is a ubiquitous mechanism for controlling molecular assembly in biological systems. However, achieving predictable reversibility in artificial two-dimensional (2D) materials remains a significant challenge. Here, we use an external electric field (EEF) at the solid/liquid interface to trigger the switching of H-bond-linked 2D networks using a scanning tunneling microscope. Assisted by density functional theory and molecular dynamics simulations, we systematically vary the molecule-to-molecule interactions, i.e., the hydrogen-bonding strength, as well as the molecule-to-substrate interactions to analyze the EEF switching effect. By tuning the building block’s hydrogen-bonding ability (carboxylic acids vs aldehydes) and substrate nature and charge (graphite, graphene/Cu, graphene/SiO2), we induce or freeze the switching properties and control the final polymorphic output in the 2D network. Our results indicate that the switching ability is not inherent to any particular building block but instead relies on a synergistic combination of the relative adsorbate/adsorbate and absorbate/substrate energetic contributions under surface polarization. Furthermore, we describe the dynamics of the switching mechanism based on the rotation of carboxylic groups and proton exchange, which generate the polarizable species that are influenced by the EEF. This work provides insights into the design and control of reversible molecular assembly in 2D materials, with potential applications in a wide range of fields, including sensors and electronics.
Fil: Cometto, Fernando Pablo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Investigaciones en Físico-química de Córdoba. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Instituto de Investigaciones en Físico-química de Córdoba; Argentina
Fil: Arisnabarreta, Nicolás. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Investigaciones en Físico-química de Córdoba. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Instituto de Investigaciones en Físico-química de Córdoba; Argentina
Fil: Vanta, Radovan. No especifíca;
Fil: Jacquelin, Daniela Karina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Investigaciones en Físico-química de Córdoba. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Instituto de Investigaciones en Físico-química de Córdoba; Argentina
Fil: Vyas, Vijay. No especifíca;
Fil: Lotsch, Bettina V.. Universitat Technical Zu Munich; Alemania
Fil: Paredes Olivera, Patricia. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Investigaciones en Físico-química de Córdoba. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Instituto de Investigaciones en Físico-química de Córdoba; Argentina
Fil: Patrito, Eduardo Martin. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Investigaciones en Físico-química de Córdoba. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Instituto de Investigaciones en Físico-química de Córdoba; Argentina
Fil: Lingenfelder, Magalí Alejandra. No especifíca;
Materia
SELF-ASSEMBLY
SCANNING TUNNELING MICROSCOPY
EXTERNAL ELECTRIC FIELD
PHASE BEHAVIOR
Nivel de accesibilidad
acceso abierto
Condiciones de uso
https://creativecommons.org/licenses/by/2.5/ar/
Repositorio
CONICET Digital (CONICET)
Institución
Consejo Nacional de Investigaciones Científicas y Técnicas
OAI Identificador
oai:ri.conicet.gov.ar:11336/259133
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/259133
network_acronym_str CONICETDig
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network_name_str CONICET Digital (CONICET)
spelling Rational Design of 2D Supramolecular Networks Switchable by External Electric FieldsCometto, Fernando PabloArisnabarreta, NicolásVanta, RadovanJacquelin, Daniela KarinaVyas, VijayLotsch, Bettina V.Paredes Olivera, PatriciaPatrito, Eduardo MartinLingenfelder, Magalí AlejandraSELF-ASSEMBLYSCANNING TUNNELING MICROSCOPYEXTERNAL ELECTRIC FIELDPHASE BEHAVIORhttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1The reversible formation of hydrogen bonds is a ubiquitous mechanism for controlling molecular assembly in biological systems. However, achieving predictable reversibility in artificial two-dimensional (2D) materials remains a significant challenge. Here, we use an external electric field (EEF) at the solid/liquid interface to trigger the switching of H-bond-linked 2D networks using a scanning tunneling microscope. Assisted by density functional theory and molecular dynamics simulations, we systematically vary the molecule-to-molecule interactions, i.e., the hydrogen-bonding strength, as well as the molecule-to-substrate interactions to analyze the EEF switching effect. By tuning the building block’s hydrogen-bonding ability (carboxylic acids vs aldehydes) and substrate nature and charge (graphite, graphene/Cu, graphene/SiO2), we induce or freeze the switching properties and control the final polymorphic output in the 2D network. Our results indicate that the switching ability is not inherent to any particular building block but instead relies on a synergistic combination of the relative adsorbate/adsorbate and absorbate/substrate energetic contributions under surface polarization. Furthermore, we describe the dynamics of the switching mechanism based on the rotation of carboxylic groups and proton exchange, which generate the polarizable species that are influenced by the EEF. This work provides insights into the design and control of reversible molecular assembly in 2D materials, with potential applications in a wide range of fields, including sensors and electronics.Fil: Cometto, Fernando Pablo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Investigaciones en Físico-química de Córdoba. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Instituto de Investigaciones en Físico-química de Córdoba; ArgentinaFil: Arisnabarreta, Nicolás. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Investigaciones en Físico-química de Córdoba. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Instituto de Investigaciones en Físico-química de Córdoba; ArgentinaFil: Vanta, Radovan. No especifíca;Fil: Jacquelin, Daniela Karina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Investigaciones en Físico-química de Córdoba. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Instituto de Investigaciones en Físico-química de Córdoba; ArgentinaFil: Vyas, Vijay. No especifíca;Fil: Lotsch, Bettina V.. Universitat Technical Zu Munich; AlemaniaFil: Paredes Olivera, Patricia. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Investigaciones en Físico-química de Córdoba. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Instituto de Investigaciones en Físico-química de Córdoba; ArgentinaFil: Patrito, Eduardo Martin. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Investigaciones en Físico-química de Córdoba. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Instituto de Investigaciones en Físico-química de Córdoba; ArgentinaFil: Lingenfelder, Magalí Alejandra. No especifíca;American Chemical Society2024-01info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfapplication/pdfapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/259133Cometto, Fernando Pablo; Arisnabarreta, Nicolás; Vanta, Radovan; Jacquelin, Daniela Karina; Vyas, Vijay ; et al.; Rational Design of 2D Supramolecular Networks Switchable by External Electric Fields; American Chemical Society; ACS Nano; 2024; 5; 1-2024; 4287-42961936-0851CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/doi/10.1021/acsnano.3c09775info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-29T09:37:50Zoai:ri.conicet.gov.ar:11336/259133instacron: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 09:37:50.539CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Rational Design of 2D Supramolecular Networks Switchable by External Electric Fields
title Rational Design of 2D Supramolecular Networks Switchable by External Electric Fields
spellingShingle Rational Design of 2D Supramolecular Networks Switchable by External Electric Fields
Cometto, Fernando Pablo
SELF-ASSEMBLY
SCANNING TUNNELING MICROSCOPY
EXTERNAL ELECTRIC FIELD
PHASE BEHAVIOR
title_short Rational Design of 2D Supramolecular Networks Switchable by External Electric Fields
title_full Rational Design of 2D Supramolecular Networks Switchable by External Electric Fields
title_fullStr Rational Design of 2D Supramolecular Networks Switchable by External Electric Fields
title_full_unstemmed Rational Design of 2D Supramolecular Networks Switchable by External Electric Fields
title_sort Rational Design of 2D Supramolecular Networks Switchable by External Electric Fields
dc.creator.none.fl_str_mv Cometto, Fernando Pablo
Arisnabarreta, Nicolás
Vanta, Radovan
Jacquelin, Daniela Karina
Vyas, Vijay
Lotsch, Bettina V.
Paredes Olivera, Patricia
Patrito, Eduardo Martin
Lingenfelder, Magalí Alejandra
author Cometto, Fernando Pablo
author_facet Cometto, Fernando Pablo
Arisnabarreta, Nicolás
Vanta, Radovan
Jacquelin, Daniela Karina
Vyas, Vijay
Lotsch, Bettina V.
Paredes Olivera, Patricia
Patrito, Eduardo Martin
Lingenfelder, Magalí Alejandra
author_role author
author2 Arisnabarreta, Nicolás
Vanta, Radovan
Jacquelin, Daniela Karina
Vyas, Vijay
Lotsch, Bettina V.
Paredes Olivera, Patricia
Patrito, Eduardo Martin
Lingenfelder, Magalí Alejandra
author2_role author
author
author
author
author
author
author
author
dc.subject.none.fl_str_mv SELF-ASSEMBLY
SCANNING TUNNELING MICROSCOPY
EXTERNAL ELECTRIC FIELD
PHASE BEHAVIOR
topic SELF-ASSEMBLY
SCANNING TUNNELING MICROSCOPY
EXTERNAL ELECTRIC FIELD
PHASE BEHAVIOR
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv The reversible formation of hydrogen bonds is a ubiquitous mechanism for controlling molecular assembly in biological systems. However, achieving predictable reversibility in artificial two-dimensional (2D) materials remains a significant challenge. Here, we use an external electric field (EEF) at the solid/liquid interface to trigger the switching of H-bond-linked 2D networks using a scanning tunneling microscope. Assisted by density functional theory and molecular dynamics simulations, we systematically vary the molecule-to-molecule interactions, i.e., the hydrogen-bonding strength, as well as the molecule-to-substrate interactions to analyze the EEF switching effect. By tuning the building block’s hydrogen-bonding ability (carboxylic acids vs aldehydes) and substrate nature and charge (graphite, graphene/Cu, graphene/SiO2), we induce or freeze the switching properties and control the final polymorphic output in the 2D network. Our results indicate that the switching ability is not inherent to any particular building block but instead relies on a synergistic combination of the relative adsorbate/adsorbate and absorbate/substrate energetic contributions under surface polarization. Furthermore, we describe the dynamics of the switching mechanism based on the rotation of carboxylic groups and proton exchange, which generate the polarizable species that are influenced by the EEF. This work provides insights into the design and control of reversible molecular assembly in 2D materials, with potential applications in a wide range of fields, including sensors and electronics.
Fil: Cometto, Fernando Pablo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Investigaciones en Físico-química de Córdoba. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Instituto de Investigaciones en Físico-química de Córdoba; Argentina
Fil: Arisnabarreta, Nicolás. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Investigaciones en Físico-química de Córdoba. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Instituto de Investigaciones en Físico-química de Córdoba; Argentina
Fil: Vanta, Radovan. No especifíca;
Fil: Jacquelin, Daniela Karina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Investigaciones en Físico-química de Córdoba. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Instituto de Investigaciones en Físico-química de Córdoba; Argentina
Fil: Vyas, Vijay. No especifíca;
Fil: Lotsch, Bettina V.. Universitat Technical Zu Munich; Alemania
Fil: Paredes Olivera, Patricia. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Investigaciones en Físico-química de Córdoba. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Instituto de Investigaciones en Físico-química de Córdoba; Argentina
Fil: Patrito, Eduardo Martin. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Investigaciones en Físico-química de Córdoba. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Instituto de Investigaciones en Físico-química de Córdoba; Argentina
Fil: Lingenfelder, Magalí Alejandra. No especifíca;
description The reversible formation of hydrogen bonds is a ubiquitous mechanism for controlling molecular assembly in biological systems. However, achieving predictable reversibility in artificial two-dimensional (2D) materials remains a significant challenge. Here, we use an external electric field (EEF) at the solid/liquid interface to trigger the switching of H-bond-linked 2D networks using a scanning tunneling microscope. Assisted by density functional theory and molecular dynamics simulations, we systematically vary the molecule-to-molecule interactions, i.e., the hydrogen-bonding strength, as well as the molecule-to-substrate interactions to analyze the EEF switching effect. By tuning the building block’s hydrogen-bonding ability (carboxylic acids vs aldehydes) and substrate nature and charge (graphite, graphene/Cu, graphene/SiO2), we induce or freeze the switching properties and control the final polymorphic output in the 2D network. Our results indicate that the switching ability is not inherent to any particular building block but instead relies on a synergistic combination of the relative adsorbate/adsorbate and absorbate/substrate energetic contributions under surface polarization. Furthermore, we describe the dynamics of the switching mechanism based on the rotation of carboxylic groups and proton exchange, which generate the polarizable species that are influenced by the EEF. This work provides insights into the design and control of reversible molecular assembly in 2D materials, with potential applications in a wide range of fields, including sensors and electronics.
publishDate 2024
dc.date.none.fl_str_mv 2024-01
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/11336/259133
Cometto, Fernando Pablo; Arisnabarreta, Nicolás; Vanta, Radovan; Jacquelin, Daniela Karina; Vyas, Vijay ; et al.; Rational Design of 2D Supramolecular Networks Switchable by External Electric Fields; American Chemical Society; ACS Nano; 2024; 5; 1-2024; 4287-4296
1936-0851
CONICET Digital
CONICET
url http://hdl.handle.net/11336/259133
identifier_str_mv Cometto, Fernando Pablo; Arisnabarreta, Nicolás; Vanta, Radovan; Jacquelin, Daniela Karina; Vyas, Vijay ; et al.; Rational Design of 2D Supramolecular Networks Switchable by External Electric Fields; American Chemical Society; ACS Nano; 2024; 5; 1-2024; 4287-4296
1936-0851
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/doi/10.1021/acsnano.3c09775
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
application/pdf
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
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score 13.070432

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