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Atomically thin PtSe2 films have attracted extensive research interests forpotential applications in high-speed electronics, spintronics andphotodetectors. Obtaining high quality, single crystalline thin films withlarge size is critical. Here we report the first successful layer-by-layergrowth of high quality PtSe2 films by molecular beam epitaxy. Atomically thinfilms from 1 ML to 22 ML have been grown and characterized by low-energyelectron diffraction, Raman spectroscopy and X-ray photoemission spectroscopy.Moreover, a systematic thickness dependent study of the electronic structure isrevealed by angle-resolved photoemission spectroscopy (ARPES), and helical spintexture is revealed by spin-ARPES. Our work provides new opportunities forgrowing large size single crystalline films for investigating the physicalproperties and potential applications of PtSe2.

High quality atomically thin PtSe2 films grown by molecular beam epitaxy