Emergent Spin Frustration in Neutral Mixed-Valence 2D Conjugated Polymers : A Potential Quantum Materials Platform
Alcón, Isaac (Institut Català de Nanociència i Nanotecnologia)
Ribas-Ariño, Jordi (Universitat de Barcelona. Departament de Ciència de Materials i Química Física)
Moreira, Ibério de P.R. (Universitat de Barcelona. Departament de Ciència de Materials i Química Física)
Bromley, Stefan (Institució Catalana de Recerca i Estudis Avançats)

Date:	2023
Abstract:	Two-dimensional conjugated polymers (2DCPs)-organic 2D materials composed of arrays of carbon sp 2 centers connected by π-conjugated linkers-are attracting increasing attention due to their potential applications in device technologies. This interest stems from the ability of 2DCPs to host a range of correlated electronic and magnetic states (e. g. , Mott insulators). Substitution of all carbon sp 2 centers in 2DCPs by nitrogen or boron results in diamagnetic insulating states. Partial substitution of C sp 2 centers by B or N atoms has not yet been considered for extended 2DCPs but has been extensively studied in the analogous neutral mixed-valence molecular systems. Here, we employ accurate first-principles calculations to predict the electronic and magnetic properties of a new class of hexagonally connected neutral mixed-valence 2DCPs in which every other C sp 2 nodal center is substituted by either a N or B atom. We show that these neutral mixed-valence 2DCPs significantly energetically favor a state with emergent superexchange-mediated antiferromagnetic (AFM) interactions between C-based spin- 1 / centers on a triangular sublattice. These AFM interactions are surprisingly strong and comparable to those in the parent compounds of cuprate superconductors. The rigid and covalently linked symmetric triangular AFM lattice in these materials thus provides a highly promising and robust basis for 2D spin frustration. As such, extended mixed-valence 2DCPs are a highly attractive platform for the future bottom-up realization of a new class of all-organic quantum materials, which could host exotic correlated electronic states (e. g. , unusual magnetic ordering, quantum spin liquids).
Grants:	Agència de Gestió d'Ajuts Universitaris i de Recerca 2021/SGR-00354 Ministerio de Ciencia e Innovación TED2021-132550B-C21 Ministerio de Economía y Competitividad SEV-2017-0706 Agencia Estatal de Investigación PID2021-127957NB-I00 Agencia Estatal de Investigación PID2020-117803GB-I00 Agencia Estatal de Investigación PID2019-109518GB-I00 Ministerio de Ciencia e Innovación FJC2019-038971-I Agencia Estatal de Investigación CEX2021-001202-M
Rights:	Aquest document està subjecte a una llicència d'ús Creative Commons. Es permet la reproducció total o parcial, la distribució, la comunicació pública de l'obra i la creació d'obres derivades, fins i tot amb finalitats comercials, sempre i quan es reconegui l'autoria de l'obra original.
Language:	Anglès
Document:	Article ; recerca ; Versió publicada
Published in:	Journal of the American Chemical Society, Vol. 145, Issue 10 (March 2023) , p. 5674-5683, ISSN 1520-5126

DOI: 10.1021/jacs.2c11185
PMID: 36877195

10 p, 4.0 MB

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Research literature > UAB research groups literature > Research Centres and Groups (research output) > Experimental sciences > Catalan Institute of Nanoscience and Nanotechnology (ICN2)
Articles > Research articles
Articles > Published articles