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-TaS2 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.