Topological Engineering of a Frustrated Antiferromagnetic Triradical in Aza-Triangulene Architectures

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Main Authors: Romero-Lara, Francisco, Vilas-Varela, Manuel, Ortiz, Ricardo, Kumar, Manish, Vegliante, Alessio, Gómez-Rodrigo, Lucía, Calupitan, Jan Patrick, Soler, Diego, Friedrich, Nikas, Wang, Dongfei, Ortuzar, Jon, Trivini, Stefano, Schulz, Fabian, Frederiksen, Thomas, Jelínek, Pavel, Peña, Diego, Pascual, Jose Ignacio
Format: Preprint
Published: 2025
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author Romero-Lara, Francisco
Vilas-Varela, Manuel
Ortiz, Ricardo
Kumar, Manish
Vegliante, Alessio
Gómez-Rodrigo, Lucía
Calupitan, Jan Patrick
Soler, Diego
Friedrich, Nikas
Wang, Dongfei
Ortuzar, Jon
Trivini, Stefano
Schulz, Fabian
Frederiksen, Thomas
Jelínek, Pavel
Peña, Diego
Pascual, Jose Ignacio
author_facet Romero-Lara, Francisco
Vilas-Varela, Manuel
Ortiz, Ricardo
Kumar, Manish
Vegliante, Alessio
Gómez-Rodrigo, Lucía
Calupitan, Jan Patrick
Soler, Diego
Friedrich, Nikas
Wang, Dongfei
Ortuzar, Jon
Trivini, Stefano
Schulz, Fabian
Frederiksen, Thomas
Jelínek, Pavel
Peña, Diego
Pascual, Jose Ignacio
contents Open-shell nanographenes provide a versatile platform to host unconventional magnetic states within their π-conjugated networks. Particularly appealing are graphene architectures that incorporate spatially separated radicals and tunable interactions, offering a scalable route toward spin-based quantum architectures. Triangulenes are ideal for this purpose, as their radical count scales with size, although strong hybridization prevents individual spin control. Here, we realize a radical reconfiguration strategy that transforms a single-radical aza-triangulene into a frustrated antiferromagnetic triradical by covalently extending it with armchair anthene moieties of increasing length. Scanning tunnelling spectroscopy reveals edge-localized Kondo resonances and a doublet-to-quartet spin excitation, evidencing the emergence of correlated spins. Multi-reference electronic-structure calculations trace the progressive increase in polyradical character with anthene length, driven by the clustering of frontier states within a narrow energy window. Consequently, the initial single-radical doublet reorganizes into a frustrated triradical with weakly coupled edge spins, a molecular analog of a three-qubit quantum register.
format Preprint
id arxiv_https___arxiv_org_abs_2512_10869
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Topological Engineering of a Frustrated Antiferromagnetic Triradical in Aza-Triangulene Architectures
Romero-Lara, Francisco
Vilas-Varela, Manuel
Ortiz, Ricardo
Kumar, Manish
Vegliante, Alessio
Gómez-Rodrigo, Lucía
Calupitan, Jan Patrick
Soler, Diego
Friedrich, Nikas
Wang, Dongfei
Ortuzar, Jon
Trivini, Stefano
Schulz, Fabian
Frederiksen, Thomas
Jelínek, Pavel
Peña, Diego
Pascual, Jose Ignacio
Mesoscale and Nanoscale Physics
Chemical Physics
Open-shell nanographenes provide a versatile platform to host unconventional magnetic states within their π-conjugated networks. Particularly appealing are graphene architectures that incorporate spatially separated radicals and tunable interactions, offering a scalable route toward spin-based quantum architectures. Triangulenes are ideal for this purpose, as their radical count scales with size, although strong hybridization prevents individual spin control. Here, we realize a radical reconfiguration strategy that transforms a single-radical aza-triangulene into a frustrated antiferromagnetic triradical by covalently extending it with armchair anthene moieties of increasing length. Scanning tunnelling spectroscopy reveals edge-localized Kondo resonances and a doublet-to-quartet spin excitation, evidencing the emergence of correlated spins. Multi-reference electronic-structure calculations trace the progressive increase in polyradical character with anthene length, driven by the clustering of frontier states within a narrow energy window. Consequently, the initial single-radical doublet reorganizes into a frustrated triradical with weakly coupled edge spins, a molecular analog of a three-qubit quantum register.
title Topological Engineering of a Frustrated Antiferromagnetic Triradical in Aza-Triangulene Architectures
topic Mesoscale and Nanoscale Physics
Chemical Physics
url https://arxiv.org/abs/2512.10869