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Hydrophobic and long-chain molecule oleylamine is used to modify the spiro-OMeTAD matrix, which is then adopted for the hole-transport layer in perovskite solar cells. It is observed that after moderate doping, the power conversion efficiency of the devices increases from 17.82 (±1.47)% to 20.68 (±0.77)%, with the optimized efficiency of 21.57% (AM 1.5G, 100 mW/cm2). The improved efficiency is ascribed to the favored charge extraction and retarded charge recombination, as reflected by transient photovoltage/photocurrent curves and impedance spectroscopy measurement. In addition, the grazing incidence photoluminescence spectrum reveals that oleylamine doping causes a blue shift of the luminescence peak of the surface layer of the halide perovskite film, while the Mott−Schottky study observes 100 mV increment in the built-in potential, both of which indicate possible defect passivation behavior on the perovskite. Moreover, an accelerated damp test observes that moisture resistance of the device is also upgraded, which is due to the improved hydrophobicity of the spiro-OMeTAD matrix. 

X-ray photoelectron spectroscopy (XPS), ultraviolet photoelectron spectroscopy (UPS), atomic force microscopy (AFM) and X-ray diffraction (XRD) were applied to investigate the electronic structure and molecular packing of C8-BTBT on HOPG with an ultrathin C 60 interlayer. It was found that C8-BTBT displays a Vollmer–Weber (V–W) growth mode on HOPG, with an ultrathin C 60 interlayer (0.7 nm). Compared to the uniform lying-down growth mode as directly grown on HOPG, the C8-BTBT molecules here adopt a lying-down orientation at low coverage with some small tilt angles because the π–π interaction between C8-BTBT and HOPG is partly disturbed by the C 60 interlayer, delivering a higher highest occupied molecular orbital (HOMO) in C8-BTBT. An interface dipole of 0.14 eV is observed due to electron transport from C8-BTBT to C 60 . The upward and downward band bending in C8-BTBT and C 60 , respectively, near the C8-BTBT/C 60 interface reduces the hole transport barrier at the interface, facilitating the hole injection from C 60 to C8-BTBT, while a large electron transfer barrier from C 60 to C8-BTBT is detected at this interface, which effectively limits electron injection from C 60 to C8-BTBT. The HOMO of C8-BTBT near the interface is largely lifted up by the C 60 insertion layer, which causes a p-doping effect and increases the hole mobility in C8-BTBT. Furthermore, owing to the lowest occupied molecular orbital (LUMO) of C 60 residing in the gap of C8-BTBT, charge transfer occurs between C 60 and the trap states in C8-BTBT to effectively passivate the trapping states. Our efforts aid a better understanding of the electron structure and film growth of anisotropic molecules and provide a useful strategy to improve the performance of C8-BTBT-based devices.