Tailored Vapor Deposition Unlocks Large-Grain, Wafer-Scale Epitaxial Growth of 2D Magnetic CrCl3

Abstract

Two-dimensional magnetic materials (2D-MM) are an exciting playground for fundamental research, and for spintronics and quantum sensing. However, their large-grain large-area synthesis using scalable vapour deposition methods is still an unsolved challenge. Here, we develop a tailored approach for centimetre-scale growth of semiconducting 2D-MM CrCl3 films on mica substrate, via physical vapour transport deposition. A controlled synthesis protocol, enabled via innovations concerning light management, very-high carrier-gas flow, precursor flux, and oxygen/moisture removal, is critical for wafer-scale growth. Optical, stoichiometric, structural, and magnetic characterization identify crystalline, phase-pure 2D-MM CrCl3. Substrate temperature tunes thickness of films from few-layers to tens of nanometres. Further, selective-area growth and large-area transfer are demonstrated. Substrate-dependent growth features are explained by density functional theory and state-of-the-art machine learning interatomic potential-based atomic-scale simulations. This scalable vapour deposition approach can be applied for growth of several 2D-MM, and low growth temperature (~500 C) will enable creation of hybrid heterostructures.

62 pages, 5 figures (main text), 15 figures and 3 tables (supplementary)

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