layer-modulated magnetism and robust stability in air. These properties make it a promising candidate in various fields like electronics, [1][2][3][4][5] optoelectronics, [6][7][8][9][10][11][12][13] spintronics, [14] catalysis, [15] micro-electromechanics, [16] and sensing. [6,17,18] Monolayer or few-layer PtSe 2 can be synthesized by different methods, such as direct selenization of Pt films at a low temperature (≤400 °C), [3,4,6,8,19] which makes it scalable and compatible with current silicon chip fabrication technology, molecular beam epitaxy (MBE), [16,20,21] chemical vapor deposition (CVD), [5,22] and chemical vapor transport (CVT). [1,23] While PtSe 2 is a semimetal in bulk, [23] it becomes a semiconductor when thinned down to a few layers, due to the quantum confinement effect. [3] Its electronic structure has been studied by angle-resolved photoemission spectroscopy (ARPES), which reveals the semiconducting property of monolayer PtSe 2 with the top of its valence band located at 1.2 eV below the Fermi level. [17,20] Complemented by density functional theory (DFT) calculations under the localizeddensity approximation (DFT-LDA), monolayer PtSe 2 is determined to be an indirect-gap semiconductor (≈1.2 eV). [17] Besides the first layer, PtSe 2 remains semiconducting at the thickness of bilayer with a significantly reduced gap of 0.21 eV and becomes semimetallic from the third layer, as predicted by DFT-LDA calculations. [17,24] However, the ARPES measurement only gives the area-average information of the band structure below the Fermi level and its results are subject to the crystal size and quality. For