Fully characterized linear magnetoelectric response of 2D monolayers from high-throughput first-principles calculations

TL;DR

This study uses high-throughput first-principles calculations to identify and fully characterize the linear magnetoelectric response in a large set of 2D monolayers, revealing materials with responses surpassing known bulk compounds.

Contribution

It provides a comprehensive computational screening and detailed analysis of the linear magnetoelectric effect in 2D monolayers, including all relevant physical contributions.

Findings

AFM monolayers generally exhibit larger ME responses than FM ones.

AFM Mn2SI2 shows the strongest ME response, about 580 ps/m.

Some compounds display antiferroic tensor entries indicating antimagnetoelectricity.

Abstract

We screen 4784 stable monolayers from the Computational 2D Materials Database (C2DB) and identify 57 ferromagnetic (FM) and 67 antiferromagnetic (AFM) compounds that should exhibit linear magnetoelectric (ME) effects. Using density functional theory, we compute contributions from the spin and orbital angular momentum as well as lattice-mediated and clamped-ion analogs to fully characterize the linear ME tensor in the static limit. We observe a general trend that AFM ordering gives rise to a larger ME response compared to FM ordered monolayers. Using a typical van der Waals interlayer distance, we find that AFM $\mathrm{Mn}_2\mathrm{SI}_2$ exhibits the strongest component of linear ME response, providing approximately 580 ps/m. This is two orders of magnitude greater than in prototypical $\mathrm{Cr}_2\mathrm{O}_3$ but comparable to the largest ME response measured in bulk $\mathrm{TbPO}_4$ (280-740 ps/m). We also search for antimagnetoelectricity and find a number of FM and AFM compounds with antiferroic tensor entries. By demonstration of select examples and analysis of our full data set, we argue that inclusion of all contributions (spin, orbital, lattice-mediated and clamped-ion) is of crucial importance for reliable predictions of the total ME response.