“…[1][2][3][4][5] Being a heavy element with unique and anomalous electronic properties, the semimetal bismuth (Bi) is one of the most extensively studied materials and has played an exceptional role in revealing many interesting phenomena in solid-state physics. [6][7][8][9][10][11][12] In particular, ultrathin Bi films have provided a representative platform for fundamental and technological explorations through delicate tailoring of their atomic and electronic structures, [13][14][15][16][17][18][19][20][21] interfacial structure, [2,3,[22][23][24][25] charge doping, [21,26] etc. When Bi is deposited on alternative substrates with a few-layer atomic thickness, such as Si(111), [27] highly oriented pyrolytic graphite (HOPG), [13,22,28] epitaxial graphene, [23,29] NbSe 2 , [21,26] and ferromagnetic Fe 3 GeTe 2 , [25] Bi normally forms Bi(110)-oriented thin films.…”