“…Controlling and manipulating electron spins in nonmagnetic semiconductor materials with a strong spin orbit interaction (SOI) have received intense interest in the field of spintronics. − Bismuth oxyselenide (Bi 2 O 2 Se) is a two-dimensional (2D) layered semiconductor material with high electron Hall mobility and good environmental stability, which exhibits excellent electron transport and optical properties for photoelectric applications. − Recently, the existence of strong SOI has been experimentally demonstrated in Bi 2 O 2 Se nanosheets, which inaugurates the possibility of Bi 2 O 2 Se for application in spintronics and quantum devices. , Previous research has established that Bi 2 O 2 Se is composed of Bi–O 2 –Bi trilayers with positively charged and Se atomic layers with a compensating negative charge, which may lead to the metallic Rashba-split surface states on the polar surfaces. − These surface states stem from huge potential bending, positive or negative, depending on surface polarity, and reside partially in the bulk band gap, leaving appropriate space for multifunctional electrical tuning. , However, so far, there is no method that can differentiate between the Bi- or Se-terminated surfaces. Since the lattice polarity is a very important issue for the study of Bi 2 O 2 Se, which will lead to different surface electronic structures, it is necessary to carry out systematic investigations to distinguish the lattice polarity of Bi 2 O 2 Se.…”