摘要： CuSCN has been employed as the hole transporting material for solar cells and it is established to offer superior power conversion efficiencies and stabilities of the perovskite solar cell. In this manuscript, we carry out first principles calculations to understand the structures and properties CuSCN surfaces in the presence of small molecules that are common in the solution processable solar cells. The molecular adsorbates include additives, precursors and solvents to synthesize the halide perovskite solar cell components such as methylammonium iodide (MAI), lead iodide (PbI2), acetonitrile, chloroform, dimethylformamide (DMF), dimethylsulfoxide (DMSO), methanol and ethanol. The study suggests that the CuSCN surfaces interact with these additive molecules in various degrees and such adsorption is strongly dependent on the CuSCN surface directions. The presence of the PbI2 moiety leads to additional empty states inside the band gap of CuSCN. The presence of the molecular adsorbates impacts on the electronic and optical properties of the CuSCN surfaces, and further additive-based interfacial engineering approach of the perovskite/CuSCN system is called for. This study paves the way toward the fundamental understanding of the CuSCN surfaces toward optoelectronic applications.