Direct covalent grafting of an organic radical core on gold and silver

The functionalisation of surfaces with organic radicals, such as perchlorotriphenylmethyl (PTM) radicals or tris(2,4,6-trichloro-phenyl)methyl (TTM) radicals, is appealing for the development of molecular spintronic devices. Conventionally, organic radicals are chemisorbed to metal substrates by usi...

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Detalles Bibliográficos
Autores: Ajayakumar, Murugan, Alcón, Isaac, Bromley, Stefan T., Veciana, Jaume, Rovira, Concepció, Mas Torrent, Marta
Tipo de recurso: artículo
Estado:Versión publicada
Fecha de publicación:2017
País:España
Institución:Consejo Superior de Investigaciones Científicas (CSIC)
Repositorio:DIGITAL.CSIC. Repositorio Institucional del CSIC
OAI Identifier:oai:digital.csic.es:10261/162056
Acceso en línea:http://hdl.handle.net/10261/162056
Access Level:acceso abierto
Palabra clave:Self-assembled monolayers
Energy-level alignment
Polychlorotriphenylmethyl radicals
Molecular switch
Spectroscopy
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dc.title.none.fl_str_mv Direct covalent grafting of an organic radical core on gold and silver
title Direct covalent grafting of an organic radical core on gold and silver
spellingShingle Direct covalent grafting of an organic radical core on gold and silver
Ajayakumar, Murugan
Self-assembled monolayers
Energy-level alignment
Polychlorotriphenylmethyl radicals
Molecular switch
Spectroscopy
title_short Direct covalent grafting of an organic radical core on gold and silver
title_full Direct covalent grafting of an organic radical core on gold and silver
title_fullStr Direct covalent grafting of an organic radical core on gold and silver
title_full_unstemmed Direct covalent grafting of an organic radical core on gold and silver
title_sort Direct covalent grafting of an organic radical core on gold and silver
dc.creator.none.fl_str_mv Ajayakumar, Murugan
Alcón, Isaac
Bromley, Stefan T.
Veciana, Jaume
Rovira, Concepció
Mas Torrent, Marta
author Ajayakumar, Murugan
author_facet Ajayakumar, Murugan
Alcón, Isaac
Bromley, Stefan T.
Veciana, Jaume
Rovira, Concepció
Mas Torrent, Marta
author_role author
author2 Alcón, Isaac
Bromley, Stefan T.
Veciana, Jaume
Rovira, Concepció
Mas Torrent, Marta
author2_role author
author
author
author
author
dc.contributor.none.fl_str_mv European Research Council
Centro de Investigación Biomédica en Red Bioingeniería, Biomateriales y Nanomedicina (España)
Ministerio de Economía y Competitividad (España)
Generalitat de Catalunya
European Commission
Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]
dc.subject.none.fl_str_mv Self-assembled monolayers
Energy-level alignment
Polychlorotriphenylmethyl radicals
Molecular switch
Spectroscopy
topic Self-assembled monolayers
Energy-level alignment
Polychlorotriphenylmethyl radicals
Molecular switch
Spectroscopy
description The functionalisation of surfaces with organic radicals, such as perchlorotriphenylmethyl (PTM) radicals or tris(2,4,6-trichloro-phenyl)methyl (TTM) radicals, is appealing for the development of molecular spintronic devices. Conventionally, organic radicals are chemisorbed to metal substrates by using long alkyl or aromatic spacers resulting in a weak spin–electron coupling between the radical and the substrate. To circumvent this problem, here we have employed a new design strategy for the fabrication of radical self-assembled monolayers (r-SAMs). This newly designed radical–anchor (R–A) molecule, a TTM based radical disulfide (1), can be easily synthesized and it was here characterized by electron spin resonance (ESR), cyclic voltammetry (CV) and superconducting quantum interference device magnetometry (SQUID). We have succeeded in fabricating TTM based r-SAMs by using thiolate bonds (Au–S and Ag–S) where the TTM cores are only one-atom distance from the metal surface for the first time. The resultant robust 1/Au and 1/Ag r-SAMs were well characterized, and the electrochemical and the magnetic properties were unambiguously confirmed, proving the persistence of the molecular spin.
publishDate 2017
dc.date.none.fl_str_mv 2017
2018
2018
dc.type.none.fl_str_mv info:eu-repo/semantics/article
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dc.identifier.none.fl_str_mv http://hdl.handle.net/10261/162056
url http://hdl.handle.net/10261/162056
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
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info:eu-repo/grantAgreement/EC/H2020/642196
info:eu-repo/grantAgreement/MINECO/Plan Estatal de Investigación Científica y Técnica y de Innovación 2013-2016/CTQ2013-40480- R
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dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
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dc.publisher.none.fl_str_mv Royal Society of Chemistry (UK)
publisher.none.fl_str_mv Royal Society of Chemistry (UK)
dc.source.none.fl_str_mv reponame:DIGITAL.CSIC. Repositorio Institucional del CSIC
instname:Consejo Superior de Investigaciones Científicas (CSIC)
instname_str Consejo Superior de Investigaciones Científicas (CSIC)
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spelling Direct covalent grafting of an organic radical core on gold and silverAjayakumar, MuruganAlcón, IsaacBromley, Stefan T.Veciana, JaumeRovira, ConcepcióMas Torrent, MartaSelf-assembled monolayersEnergy-level alignmentPolychlorotriphenylmethyl radicalsMolecular switchSpectroscopyThe functionalisation of surfaces with organic radicals, such as perchlorotriphenylmethyl (PTM) radicals or tris(2,4,6-trichloro-phenyl)methyl (TTM) radicals, is appealing for the development of molecular spintronic devices. Conventionally, organic radicals are chemisorbed to metal substrates by using long alkyl or aromatic spacers resulting in a weak spin–electron coupling between the radical and the substrate. To circumvent this problem, here we have employed a new design strategy for the fabrication of radical self-assembled monolayers (r-SAMs). This newly designed radical–anchor (R–A) molecule, a TTM based radical disulfide (1), can be easily synthesized and it was here characterized by electron spin resonance (ESR), cyclic voltammetry (CV) and superconducting quantum interference device magnetometry (SQUID). We have succeeded in fabricating TTM based r-SAMs by using thiolate bonds (Au–S and Ag–S) where the TTM cores are only one-atom distance from the metal surface for the first time. The resultant robust 1/Au and 1/Ag r-SAMs were well characterized, and the electrochemical and the magnetic properties were unambiguously confirmed, proving the persistence of the molecular spin.This work was funded by ERC StG 2012-306826 e-GAMES. The authors also thank ITN iSwitch 642196 project, the Networking Research Center on Bioengineering, Biomaterials and Nanomedicine (CIBER-BBN), DGI (Spain) BE-WELL CTQ2013-40480- R and FANCY CTQ2016-80030-R, and Generalitat de Catalunya 2014-SGR-17. The authors also acknowledge the Spanish Ministry of Economy and Competitiveness, through the “Severo Ochoa” Programme for Centres of Excellence in R&D (SEV-2015- 0496). We thank Dr V. Lloveras for ESR spectroscopy characterization, Mr A. Bernab´e for MALDI-TOF measurements and Dr G. Sauthier from ICN2 for XPS and UPS measurements. We also thank Dr N. Crivillers for useful discussions. S. T. B. and I. A. acknowledge support from the Spanish MINECO grant CTQ2015-64618-R grant and, in part, by Generalitat de Catalunya grants 2014SGR97 and XRQTC. IA acknowledges the Spanish Ministerio de Educaci´on Cultura y Deporte for a FPU PhD scholarship. Access to supercomputer resources as provided through grants from the Red Espanola de Supercomputación is also acknowledged.Peer reviewedRoyal Society of Chemistry (UK)European Research CouncilCentro de Investigación Biomédica en Red Bioingeniería, Biomateriales y Nanomedicina (España)Ministerio de Economía y Competitividad (España)Generalitat de CatalunyaEuropean CommissionConsejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]201820182017info:eu-repo/semantics/articlehttp://purl.org/coar/resource_type/c_6501Publisher's versioninfo:eu-repo/semantics/publishedVersionhttp://hdl.handle.net/10261/162056reponame:DIGITAL.CSIC. Repositorio Institucional del CSICinstname:Consejo Superior de Investigaciones Científicas (CSIC)Inglés#PLACEHOLDER_PARENT_METADATA_VALUE##PLACEHOLDER_PARENT_METADATA_VALUE##PLACEHOLDER_PARENT_METADATA_VALUE##PLACEHOLDER_PARENT_METADATA_VALUE##PLACEHOLDER_PARENT_METADATA_VALUE##PLACEHOLDER_PARENT_METADATA_VALUE#info:eu-repo/grantAgreement/EC/FP7/306826info:eu-repo/grantAgreement/EC/H2020/642196info:eu-repo/grantAgreement/MINECO/Plan Estatal de Investigación Científica y Técnica y de Innovación 2013-2016/CTQ2013-40480- Rinfo:eu-repo/grantAgreement/MINECO/Plan Estatal de Investigación Científica y Técnica y de Innovación 2013-2016/CTQ2016-80030-Rinfo:eu-repo/grantAgreement/MINECO/Plan Estatal de Investigación Científica y Técnica y de Innovación 2013-2016/SEV-2015-0496info:eu-repo/grantAgreement/MINECO/Plan Estatal de Investigación Científica y Técnica y de Innovación 2013-2016/CTQ2015-64618-Rhttp://dx.doi.org/10.1039/C7RA01686GSíinfo:eu-repo/semantics/openAccessoai:digital.csic.es:10261/1620562026-05-22T06:33:51Z
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