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Copper thiocyanate (CuSCN) and copper selenocyanate (CuSeCN) combine a high work function with a high optical transparency. To elucidate their potential as transparent hole selective materials, herein, first‐principles calculations of the structural and electronic properties are reported, with special attention to the band offsets with crystalline Si and hybrid perovskites (CH3NH3PbI3, CH3NH3PbBr...
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