Superexchange Mechanism in Coupled Triangulenes Forming Spin-1 Chains.

Saleem, Yasser; Steenbock, Torben; Alhadi, Emha Riyadhul Jinan; Pasek, Weronika; Bester, Gabriel; Potasz, Pawel · Nano Lett · 2024

basic_science · Level V

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Abstract

We show that the origin of the antiferromagnetic coupling in spin-1 triangulene chains, which were recently synthesized and measured by Mishra et al. ( <i>Nature</i> 2021, 598, 287-292), originates from a superexchange mechanism. This process, mediated by intertriangulene states, opens the possibility to control parameters in the effective bilinear-biquadratic spin model. We start from the derivation of an effective tight-binding model for triangulene chains using a combination of tight-binding and Hartree-Fock methods fitted to hybrid density functional theory results. Next, correlation effects are investigated within the configuration interaction method. Our low-energy many-body spectrum for <i>N</i><sub>Tr</sub> = 2 and <i>N</i><sub>Tr</sub> = 4 triangulene chains agree well with the bilinear-biquadratic spin-1 chain antiferromagnetic model when indirect coupling processes and superexchange coupling between triangulene spins are taken into account.