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Poly(3,4‐ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) is a popular hole transport material in perovskite solar cells (PSCs). However, the devices with PEDOT:PSS exhibit large open‐circuit voltage (Voc) loss and low efficiency, which is attributed to mismatched energy level alignment and the poor interface of PEDOT:PSS and perovskite. Here, three polymer analogues to polyaniline (PANI), PANI–carbazole (P1), PANI–phenoxazine (P2), and PANI–phenothiazine (P3) are designed with different energy levels to modify the interface between PEDOT:PSS and the perovskite layer and improve the device performance. The effects of the polymers on the device performance are demonstrated by evaluating the work function adjustment, perovskite growth control, and interface modification in MAPbI3‐based PSCs. Low bandgap Sn–Pb‐based PSCs are also fabricated to confirm the effects of the polymers. Three effects are evaluated through the comparison study of PEDOT:PSS‐based organic solar cells and MAPbI3 PSCs based on the PEDOT:PSS modified by P1, P2, and P3. The order of contribution for the three effects is work function adjustment > surface modification > perovskite growth control. MAPbI3 PSCs modified with P2 exhibit a high Voc of 1.13 V and a high‐power conversion efficiency of 21.06%. This work provides the fundamental understanding of the interface passivation effects for PEDOT:PSS‐based optoelectronic devices.

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The power conversion efficiency (PCE) of perovskite solar cells (PSCs) has increased and levels with silicon solar cells; however, their commercialization has not yet been realized because of their poor long-term stability. One of the primary causes of the instability of PSC devices is the large concentration of defects in the polycrystalline perovskite film. Such defects limit the device performance besides triggering hysteresis and device instability. In this study, tetradodecylammonium bromide (TDDAB) was used as a postsurface modifier to suppress the density of defects from the mixed perovskite film (CsFAMA). X-ray photoelectron spectroscopy (XPS) and Fourier transform infrared spectroscopy (FTIR) analyses validated that TDDAB binds to the mixed perovskite through hydrogen bonding. The X-ray diffraction (XRD) and two-dimensional grazing incidence wide-angle X-ray scattering (2D GIWAXS) study uncovered that the TDDAB modification formed a capping layer of (TDDA)2PbI1.66Br2.34 on the surface of the three-dimensional (3D) perovskite. The single charge transport device prepared from the TDDAB-modified perovskite film revealed that both the electron and hole defects were considerably repressed due to the modification. Consequently, the modified device displayed a champion PCE of 21.33%. The TDDAB surface treatment not only enhances the PCE but the bulky cation of the TDDAB also forms a hydrophobic capping surface (water contact angle of 93.39°) and safeguards the underlayer perovskite from moisture. As a result, the modified PSC has exhibited almost no performance loss after 30 days in air (RH ≈ 40%).

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