Giant Thickness‐Tunable Bandgap and Robust Air Stability of 2D Palladium Diselenide

Uncovering the thickness-dependent electronic property and environmental stability for 2D materials are crucial issues for promoting their applications in high-performance electronic and optoelectronic devices. Herein, the extrahigh air stability and giant tunable electronic bandgap of chemical vapor deposition (CVD)-derived few-layer PdSe2 on Au foils, by using scanning tunneling microscope/spectroscopy (STM/STS), are reported. The robust stability of 2D PdSe2 is uncovered by the observation of nearly defect/adsorption-free atomic lattices on long-time air-exposed samples. A one-to-one correspondence between the electronic bandgap (from ≈1.15 to ≈0 eV) and thickness of PdSe2 /Au (from bilayer to bulk) is established. It is also revealed that few-layer semiconducting PdSe2 flakes present zero-gap edges, induced by hybridization of Pd 4d and Se 4p orbitals. This work hereby provides straightforward evidence for the thickness-tunable electronic property and air stability of 2D semiconductors, thus shedding light on their applications in next-generation electronic devices.