A dopant-free polymeric hole selective contact (HSC) layer is ubiquitous for stable perovskite solar cells (PSCs). However, the intrinsic nonwetting nature of the polymeric HSC impedes the uniform spreading of the perovskite precursor solution, generating a terrible buried interface. Here, we dexterously tackle this dilemma from the perspective of dispersive and polar component surface energies of the HSC layer. A novel triarylamine-based HSC material, poly­[bis­(4-phenyl)­(2,4-dimethoxyphenyl)­amine] (2MeO-PTAA), was designed by introducing the polar methoxy groups to the para and ortho positions of the dangling benzene. These nonsymmetrically substituted electron-donating methoxy groups enhanced the polar components of surface energy, allowing more tight interfacial contact between the HSC layer and perovskite and facilitating hole extraction. When utilized as the dopant-free HSC layer in inverted PSCs, the 2MeO-PTAA-based device with CH3NH3PbI3 as the absorber exhibited an encouraging power conversion efficiency of 20.23% and a high fill factor of 84.31% with negligible hysteresis. Finally, a revised detailed balance model was used to verify the drastically lessened surface defect-induced recombination loss and shunt resistance loss in 2MeO-PTAA-based devices. This work demonstrates a facile and efficient way to modulate the buried interface and shed light on the direction to further improve the photovoltaic performance of inverted PSCs with other types of perovskites.

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