Phase engineering of 1T$'$ and 1T CrS2 and Cr2S3 by MOCVD

Abstract

Layered Cr-chalcogenides compounds offer a rich range of crystal phases with different magnetic properties some of which have been predicted only but not experimentally verified. Here we demonstrate a previously unreported crystal phase of CrS2, namely the distorted octahedral (1T$'$) structure, synthesized via metal-organic chemical vapour deposition (MOCVD). We achieved the tuneable synthesis of either 1T$'$ or 1T phase CrS2. The structure were identified using polarized Raman spectroscopy, density functional perturbation theory (DFPT), as well as scanning electron diffraction (4D-STEM). 4D-STEM reveals that 1T$'$ crystals grow from an originally nucleated kinetically favoured 1T phase which then transform into the thermodynamically stable 1T$'$ phase. Magneto-optic Kerr imaging reveals that the 1T$'$ CrS2 crystals have soft ferromagnetic nature at low temperature. Our MOCVD growth of complex phases of 2D CrS2 with long-range magnetic order paves the way for the scalable synthesis of 2D magnets for ultrathin magnetic memories for logic-in-memory applications and spintronics.