Electronic properties of polymorphic two-dimensional layered chromium disulphide

Abstract

Two-dimensional (2D) Cr-based layered and non-layered materials such as CrI₃, Cr₂Ge₂Te₆, Cr₂S₃, CrSe, and CrOX (X = Cl and Br) have attracted considerable attention due to their potential application in spintronics. Despite few experimental studies, theoretical studies reported that 2D chromium dichalcogenide (CrS₂) materials show unique properties such as valley polarization, piezoelectric coupling, and phase dependent intrinsic magnetic properties. Here, we report for the first time the synthesis of 2D layered CrS₂ flakes down to the monolayer via the chemical vapor deposition (CVD) method, its phase structures and electronic properties. We observed the 2H, 1T, and 1T' phases coexisting in CVD grown monolayer CrS₂. The formation of 1T' phases from 1T phases is described by dimerization of metal atoms at room temperature according to our molecular dynamics studies. The coexistence of 1T and 1T' phases with 2H phases is referred to as the 1T and 1T' puddling phenomenon. We theoretically showed that the monolayer 2H-CrS₂ is a direct bandgap semiconductor with a gap of approximately 0.95 eV predicted by the PBE functional, while the 1T- and 1T'-CrS₂ are metallic and semi-metallic with approximately 10 meV gap, respectively. Furthermore, 2H CrS₂ exhibits nonmagnetic semiconducting properties while for ferromagnetic spin configuration, the 1T and 1T' CrS₂ show magnetic characteristics with 0.531μ_B and 2.206μ_B magnetic moment per Cr atom respectively, for ferromagnetic spin configuration as predicted from DFT+U calculation. Importantly, CrS₂-based field-effect transistors exhibit a p-type behavior. Our study would stimulate further exploration of 2D layered CrS₂ with astonishing properties and open up a whole new avenue for the urgent need for developing multifunctional 2D materials for nanoelectronics, valleytronics, and spintronics.