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.
@article{arxiv.2509.07899,
title = {Phase engineering of 1T$'$ and 1T CrS2 and Cr2S3 by MOCVD},
author = {Haoyu Bai and Gareth R. M Tainton and Mauro Och and Max Rimmer and Indrajit Maity and Filippo Mione and Khagesh Tanwar and Rongsheng Cai and Joseph Parker and Kho Zhiquan and Ercin C Duran and Evan Tillotson and Sam Sullivan-Allsop and Alexander Eggeman and Siyuan Deng and Dan Bromley and Jack N. Carter-Gartside and Alex Vanstone and Sandrine Heutz and Will R. Branford and Efrén Navarro-Moratalla and Johannes C. Lischner and Sarah Haigh and Cecilia Mattevi},
journal= {arXiv preprint arXiv:2509.07899},
year = {2025}
}