“…4 Experimentally, valley splitting has been observed by magnetic field in some 2D materials, such as WSe 2 , VS 2 and MoS 2 . [5][6][7] Recently, some 2H phase Fe-group compounds were found to generate a large spontaneous VP, such as FeX 2 (X = Cl, Br, I), [8][9][10][11][12] FeClF, 13 FeClBr, 14 RuBr 2 , [15][16][17] RuCl 2 , 18 RuClBr, 19 Ru(OH) 2 , 20 OsBr 2 , 21 and OsClBr. 22 Here, the VBM and CBM are both located at the K/K 0 point, where the VP can be observed in the valence band (VB), different from other 2D FV materials.…”