LAUSR

Abstract The accessible exfoliation of layered CrI3 [Nature 546 (2017) 270, Ref. 1] has inspired the upsurge of two-dimensional intrinsic magnetism, which is desirable for next generation of information technology. The underlying magnetic coupling mechanism is still in debate and their magnetic ordering temperature is far less than room temperature, which prohibits their real application. Herein, anion ion(iodine being replaced by bromine) and cation ions(Cr substituted by V/Mn) substitution are conducted using density functional theory, including both electron correlation(U) and spin-orbit coupling(SOC) effect, to provide an intuitive physical picture to understand their electronic and magnetic behavior. Our results indicate that the in-plane parameters, band gap, magnetic moment and magnetic ordering temperature can be tuned linearly via the concentration of bromine. Intriguingly, Both V and Mn substitution would give rise to half metallic character, a promising spintronic candidate. Moreover, V3+(3d2) would give rise to a V dxy–I px–Cr dxy exchange path, which is ferromagnetic, and thus hold great promise to enhance the magnetic ordering temperature (397 K) being above room temperature.