On‐Surface Synthesis of Non‐Benzenoid Nanographenes Embedding Azulene and Stone‐Wales Topologies
The incorporation of non-benzenoid motifs in graphene nanostructures significantly impacts their properties, making them attractive for applications in carbon-based electronics. However, understanding how specific nonbenzenoid structures influence their properties remains limited, and further invest...
| Autores: | , , , , , , , , , , , , , , |
|---|---|
| Tipo de documento: | artigo |
| Data de publicação: | 2024 |
| País: | España |
| Recursos: | Universidad Autónoma de Madrid |
| Repositório: | Biblos-e Archivo. Repositorio Institucional de la UAM |
| Idioma: | inglês |
| OAI Identifier: | oai:repositorio.uam.es:10486/715719 |
| Acesso em linha: | http://hdl.handle.net/10486/715719 https://dx.doi.org/10.1002/ange.202318185 |
| Access Level: | Acceso aberto |
| Palavra-chave: | Nanographenes azulene and Stone-Wales defects scanning tunnelling microscopy open-shell species oxidative ring-closure Física |
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On‐Surface Synthesis of Non‐Benzenoid Nanographenes Embedding Azulene and Stone‐Wales TopologiesBiswas, KalyanChen, QifanObermann, SebastianMa, JiMelidonie, JasonLauwaet, KoenJelínek, PavelFeng, XinliangSoler Polo, Diego ManuelBarragán, AnaSánchez Grande, AnaGallego, José M.Écija, DavidUrgel, José I.Miranda Soriano, RodolfoNanographenesazulene and Stone-Wales defectsscanning tunnelling microscopyopen-shell speciesoxidative ring-closureFísicaThe incorporation of non-benzenoid motifs in graphene nanostructures significantly impacts their properties, making them attractive for applications in carbon-based electronics. However, understanding how specific nonbenzenoid structures influence their properties remains limited, and further investigations are needed to fully comprehend their implications. Here, we report an on-surface synthetic strategy toward fabricating non-benzenoid nanographenes containing different combinations of pentagonal and heptagonal rings. Their structure and electronic properties were investigated via scanning tunneling microscopy and spectroscopy, complemented by computational investigations. After thermal activation of the precursor P on the Au(111) surface, we detected two major nanographene products. Nanographene Aa- a embeds two azulene units formed through oxidative ring-closure of methyl substituents, while Aa-s contains one azulene unit and one Stone-Wales defect, formed by the combination of oxidative ring-closure and skeletal ring-rearrangement reactions. Aa-a exhibits an antiferromagnetic ground state with the highest magnetic exchange coupling reported up to date for a non-benzenoid containing nanographene, coexisting with side-products with closed shell configurations resulted from the combination of ring-closure and ring-rearragement reactions (Ba-a, Ba-s, Bs-a and Bs-s). Our results provide insights into the single gold atom assisted synthesis of novel NGs containing nonbenzenoid motifs and their tailored electronic/magnetic propertiesThe authors acknowledge to several funding organizations for their financial support. We thank support from the ‘(MAD2D-CM)-IMDEA-Nanociencia’ project funded by Comunidad de Madrid, by the Recovery, Transformation and Resilience Plan, and by NextGenerationEU from the European Union; the QUIMTRONIC-CM project (Y2018/NMT-4783) by Comunidad de Madrid; and the Ministerio de Ciencia e Innovación for the PID2019-108532GB-I00 project. IMDEA Nanociencia also acknowledges the “Severo Ochoa” Programme for Centers of Excellence in R&D (MINECO, Grant SEV-2016-0686 and CEX2020-001039-S). We acknowledge support from the CzechNanoLab Research Infrastructure supported by MEYS CR (LM2023051) and the GACR project no. 23-05486S. Computational resources were provided by the e-INFRA CZ project (ID: 90254), supported by MEYS CR. In addition, we appreciate financial support by the EU Graphene Flagship (Graphene Core 3, 881603), the Center for Advancing Electronics Dresden (CFAED), H2020-EU.1.2.2.–FET Proactive Grant (LIGHT-CAP, 101017821) and the DFG-SNSF Joint Switzerland-German Research Project (EnhanTopo, No. 429265950). J. I. U. acknowledges the funding from the Marie Skłodowska-Curie grant agreement no. 886314, which is part of the European Union's Horizon 2020 research and innovation programme. Open Access publishing facilitated by Fyzikalni ustav Akademie ved Ceske republiky, as part of the Wiley - CzechELib agreementWiley VCH GmbHDepartamento de Física de la Materia CondensadaFacultad de Ciencias20242024-02-22research articlehttp://purl.org/coar/resource_type/c_2df8fbb1VoRhttp://purl.org/coar/version/c_970fb48d4fbd8a85info:eu-repo/semantics/articleapplication/pdfhttp://hdl.handle.net/10486/715719https://dx.doi.org/10.1002/ange.202318185reponame:Biblos-e Archivo. Repositorio Institucional de la UAMinstname:Universidad Autónoma de MadridInglésengopen accesshttp://purl.org/coar/access_right/c_abf2Attribution 4.0 Internationalhttp://creativecommons.org/licenses/by/4.0/info:eu-repo/semantics/openAccessoai:repositorio.uam.es:10486/7157192026-06-23T12:46:27Z |
| dc.title.none.fl_str_mv |
On‐Surface Synthesis of Non‐Benzenoid Nanographenes Embedding Azulene and Stone‐Wales Topologies |
| title |
On‐Surface Synthesis of Non‐Benzenoid Nanographenes Embedding Azulene and Stone‐Wales Topologies |
| spellingShingle |
On‐Surface Synthesis of Non‐Benzenoid Nanographenes Embedding Azulene and Stone‐Wales Topologies Biswas, Kalyan Nanographenes azulene and Stone-Wales defects scanning tunnelling microscopy open-shell species oxidative ring-closure Física |
| title_short |
On‐Surface Synthesis of Non‐Benzenoid Nanographenes Embedding Azulene and Stone‐Wales Topologies |
| title_full |
On‐Surface Synthesis of Non‐Benzenoid Nanographenes Embedding Azulene and Stone‐Wales Topologies |
| title_fullStr |
On‐Surface Synthesis of Non‐Benzenoid Nanographenes Embedding Azulene and Stone‐Wales Topologies |
| title_full_unstemmed |
On‐Surface Synthesis of Non‐Benzenoid Nanographenes Embedding Azulene and Stone‐Wales Topologies |
| title_sort |
On‐Surface Synthesis of Non‐Benzenoid Nanographenes Embedding Azulene and Stone‐Wales Topologies |
| dc.creator.none.fl_str_mv |
Biswas, Kalyan Chen, Qifan Obermann, Sebastian Ma, Ji Melidonie, Jason Lauwaet, Koen Jelínek, Pavel Feng, Xinliang Soler Polo, Diego Manuel Barragán, Ana Sánchez Grande, Ana Gallego, José M. Écija, David Urgel, José I. Miranda Soriano, Rodolfo |
| author |
Biswas, Kalyan |
| author_facet |
Biswas, Kalyan Chen, Qifan Obermann, Sebastian Ma, Ji Melidonie, Jason Lauwaet, Koen Jelínek, Pavel Feng, Xinliang Soler Polo, Diego Manuel Barragán, Ana Sánchez Grande, Ana Gallego, José M. Écija, David Urgel, José I. Miranda Soriano, Rodolfo |
| author_role |
author |
| author2 |
Chen, Qifan Obermann, Sebastian Ma, Ji Melidonie, Jason Lauwaet, Koen Jelínek, Pavel Feng, Xinliang Soler Polo, Diego Manuel Barragán, Ana Sánchez Grande, Ana Gallego, José M. Écija, David Urgel, José I. Miranda Soriano, Rodolfo |
| author2_role |
author author author author author author author author author author author author author author |
| dc.contributor.none.fl_str_mv |
Departamento de Física de la Materia Condensada Facultad de Ciencias |
| dc.subject.none.fl_str_mv |
Nanographenes azulene and Stone-Wales defects scanning tunnelling microscopy open-shell species oxidative ring-closure Física |
| topic |
Nanographenes azulene and Stone-Wales defects scanning tunnelling microscopy open-shell species oxidative ring-closure Física |
| description |
The incorporation of non-benzenoid motifs in graphene nanostructures significantly impacts their properties, making them attractive for applications in carbon-based electronics. However, understanding how specific nonbenzenoid structures influence their properties remains limited, and further investigations are needed to fully comprehend their implications. Here, we report an on-surface synthetic strategy toward fabricating non-benzenoid nanographenes containing different combinations of pentagonal and heptagonal rings. Their structure and electronic properties were investigated via scanning tunneling microscopy and spectroscopy, complemented by computational investigations. After thermal activation of the precursor P on the Au(111) surface, we detected two major nanographene products. Nanographene Aa- a embeds two azulene units formed through oxidative ring-closure of methyl substituents, while Aa-s contains one azulene unit and one Stone-Wales defect, formed by the combination of oxidative ring-closure and skeletal ring-rearrangement reactions. Aa-a exhibits an antiferromagnetic ground state with the highest magnetic exchange coupling reported up to date for a non-benzenoid containing nanographene, coexisting with side-products with closed shell configurations resulted from the combination of ring-closure and ring-rearragement reactions (Ba-a, Ba-s, Bs-a and Bs-s). Our results provide insights into the single gold atom assisted synthesis of novel NGs containing nonbenzenoid motifs and their tailored electronic/magnetic properties |
| publishDate |
2024 |
| dc.date.none.fl_str_mv |
2024 2024-02-22 |
| dc.type.none.fl_str_mv |
research article http://purl.org/coar/resource_type/c_2df8fbb1 VoR http://purl.org/coar/version/c_970fb48d4fbd8a85 |
| dc.type.openaire.fl_str_mv |
info:eu-repo/semantics/article |
| format |
article |
| dc.identifier.none.fl_str_mv |
http://hdl.handle.net/10486/715719 https://dx.doi.org/10.1002/ange.202318185 |
| url |
http://hdl.handle.net/10486/715719 https://dx.doi.org/10.1002/ange.202318185 |
| dc.language.none.fl_str_mv |
Inglés eng |
| language_invalid_str_mv |
Inglés |
| language |
eng |
| dc.rights.none.fl_str_mv |
open access http://purl.org/coar/access_right/c_abf2 Attribution 4.0 International http://creativecommons.org/licenses/by/4.0/ |
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info:eu-repo/semantics/openAccess |
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open access http://purl.org/coar/access_right/c_abf2 Attribution 4.0 International http://creativecommons.org/licenses/by/4.0/ |
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openAccess |
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application/pdf |
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Wiley VCH GmbH |
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Wiley VCH GmbH |
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reponame:Biblos-e Archivo. Repositorio Institucional de la UAM instname:Universidad Autónoma de Madrid |
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Universidad Autónoma de Madrid |
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Biblos-e Archivo. Repositorio Institucional de la UAM |
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