The power conversion efficiency (PCE) of perovskite solar cells has been showing rapid improvement in the last decade. However, still, there is an unarguable performance deficit compared with the Schockley–Queisser (SQ) limit. One of the major causes for such performance discrepancy is surface and grain boundary defects. They are a source of nonradiative recombination in the devices that not only causes performance loss but also instability of the solar cells. In this study, we employed a direct postsurface passivation strategy at mild temperatures to modify perovskite layer defects using tetraoctylammonium chloride (TOAC). The passivated perovskite layers have demonstrated extraordinary improvement in photoluminescence and charge carrier lifetimes compared to their control counterparts in both Cs0.05(FAPbI3)0.83(MAPbBr3)0.17 and MAPbI3-type perovskite layers. The investigation on electron-only and hole-only devices after TOAC treatment revealed suppressed electron and hole trap density of states. The electrochemical study demonstrated that TOAC treatment improved the charge recombination resistance of the perovskite layers and reduced the charge accumulation on the surface of perovskite films. As a result, perovskite solar cells prepared by TOAC treatment showed a champion PCE of 21.24% for the Cs0.05(FAPbI3)0.83(MAPbBr3)0.17-based device compared to 19.58% without passivation. Likewise, the PCE of MAPbI3 improved from 18.09 to 19.27% with TOAC treatment. The long-term stability of TOAC-passivated perovskite Cs0.05(FAPbI3)0.83(MAPbBr3)0.17 devices has retained over 97% of its initial performance after 720 h in air.

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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