Controlling magnetic frustration in 1T-TaS${}_2$ via Coulomb engineered long-range interactions

Abstract

Magnetic frustrations in two-dimensional materials provide a rich playground to engineer unconventional phenomena such as non-collinear magnetic order and quantum spin-liquid behavior. However, despite intense efforts, a realization of tunable frustrated magnetic order in two-dimensional materials remains an open challenge. Here we propose Coulomb engineering as a versatile strategy to tailor magnetic ground states in layered materials. Using the proximal quantum spin-liquid candidate 1T-TaS${}_2$ as an example, we show how long-range Coulomb interactions renormalize the low energy nearly flat band structure, leading to a Heisenberg model which decisively depends on the Coulomb interactions. Based on this, we show that superexchange couplings in the material can be precisely tailored by means of environmental dielectric screening, ultimately allowing to externally drive the material towards the quantum spin-liquid regime. Our results put forward Coulomb engineering as a powerful tool to manipulate magnetic properties of van der Waals materials.

6 pages, 3 figures

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Cited by in corpus (4)

• Exploring the role of nonlocal Coulomb interactions in perovskite transition metal oxides
• Doped Mott phase and charge correlations in monolayer 1T-NbSe${}_2$
• Self-doped flat band and spin-triplet superconductivity in monolayer 1T-TaSe${}_{2-x}$Te${}_x$
• Topical review: the nature of the ground state and possibility of a quantum spin liquid in 1T metal dichalcogenides