“…A significant area of research has been around identifying alternative hole transport layers (HTLs) to the commonly used organic HTLs that include (2,2′,7,7′-tetrakis(N,N-p-dimethoxyphenylamino)-9,9′-spirobifluorene (spiro-MeOTAD) and poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine] (PTAA), which yield the highest PCEs. − The need for alternatives stems from their high cost (>$170 g –1 ) and low thermal stability, which raise doubts regarding their lifetime and commercial viability. , Inorganic p-type semiconductors such as copper thiocyanate (CuSCN), copper iodide (CuI), and nickel oxide (NiO) are attractive alternatives because of their relatively low cost (<$10 g –1 ), dopant-free high conductivity, and high chemical and thermal stability. − Among these, CuSCN is the most efficient HTL for use in n-i-p architectures . The wide band gap (>3.5 eV), favorable valence-band alignment to MAPbI 3 (−5.3 eV), and high field-effect hole mobility (∼10 –2 –10 –1 cm 2 /V s) have further made CuSCN an attractive option. , Moreover, its application is limited to not only conventional (n-i-p) and inverted (p-i-n) PSCs, but also organic solar cells, thin-film transistors, and ultraviolet (UV) photodetectors. − To optimize the semiconductor for these various applications, it is essential to understand the intrinsic charge-carrier dynamics of CuSCN.…”