Single-layer CrI3 grown by molecular beam epitaxy

2020 
Abstract Single- and few-layer chromium triiodide (CrI3), which has been intensively investigated as a promising platform for two-dimensional magnetism, is usually prepared by the mechanical exfoliation. Here, we report direct growth of single-layer CrI3 using molecular beam epitaxy in ultrahigh vacuum. Scanning tunneling microscopy (STM), together with density functional theory (DFT) calculation, revealed that the iodine trimers, each of which consists of three I atoms surrounding a three-fold Cr honeycomb center, are the basic units of the topmost I layer. Different superstructures of single-layer CrI3 with periodicity around 2–4 nm were obtained on Au(111), while only the 1×1 structure was observed on the graphite substrate. At an elevated temperature of 423 K, single-layer CrI3 began to decompose and transformed into single-layer chromium diiodide. Our bias-dependent STM images suggest that the unoccupied and occupied states are spatial-separately distributed, and consistent with the results of our DFT calculation. We also discussed the role of charge distribution in the super-exchange interactions among Cr atoms in single-layer CrI3.
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