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Thickness-dependent magnetic behavior has previously been observed in chemical vapor deposition-grown chromium selenide. However, the low-dimensional structure in nonlayered chromium selenide, which plays a crucial role in determining the low-dimensional magnetic order, needs further study. Here, we report the structure-dependent magnetic properties in monolayer CrSe2 and Cr2Se3 grown by molecular beam epitaxy. In the monolayer CrSe2, 1T-CrSe2 with a lattice constant of 3.3 Å has a metallic character, coexisting with the 1T″ phase with 2 × 2 surface periodicity. Monolayer CrSe2 can be transformed into Cr2Se3 with a lattice constant of 3.6 Å by annealing at 300 °C. X-ray magnetic circular dichroism (XMCD) measurements combined with DFT calculations reveal that while the MBE-grown monolayer CrSe2 is antiferromagnetic, monolayer Cr2Se3 is ferromagnetic with a Curie temperature of ∼200 K. This work demonstrates the structural diversity in nonlayered chromium selenide and the critical effect of different structures on its electronic and magnetic properties.
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