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A deficiency in the photoelectrical dynamics at the interface due to the surface traps of the TiO2 electron transport layer (ETL) has been the critical factor for the inferiority of the power conversion efficiency (PCE) in the perovskite solar cells. Despite its excellent energy level alignment with most perovskite materials, its large density of surface defect as a result of sub lattice vacancies has been the critical hurdle for an efficient photovoltaic process in the device. Here, we report that atoms thick 2D TiS2 layer grown on the surface of a (001) faceted and single-crystalline TiO2 nanograss (NG) ETL have effectively passivated the defects, boosting the charge extractability, carrier mobility, external quantum efficiency, and the device stability. These properties allow the perovskite solar cells (PSCs) to produce a PCE as high as 18.73% with short-circuit current density (Jsc), open-circuit voltage (Voc), and fill-factor (FF) values as high as 22.04 mA/cm2, 1.13 V, and 0.752, respectively, a 3.3% improvement from the pristine TiO2-NG-based PSCs. The present approach should find an extensive application for controlling the photoelectrical dynamic deficiency in perovskite solar cells.

The efficient electron transfer at the interface of the electron transport layer (ETL) and perovskite, and the transportation along the ETL and collection at the electrode are characteristics that are critically governed by the properties of the ETL. Both characteristics are fundamental for the fabrication of high-performance perovskite solar cells (PSC). So far, mesoporous TiO2 might be considered a versatile ETL as its structure can provide an enormous heterojunction with the perovskite absorber. However, its inert (101) pore facet, massive dead-end pore structure, and extensive grain boundary with the underlying layers in the PSC device have made them unlikely to meet those basic criteria. Here, we have come up with a new design of TiO2 ETL that provides a high carrier dynamic in the device. It is a 3 nm thick high-energy (001) faceted single-crystalline nanograss-like structure (TNG) that is vertically grown on the ITO surface. With these unique structural properties, we achieved an enhanced carrier extraction from the perovskite layer, transportation along the ETL and collection at the electrode. Our results indicate that the charge-transfer dynamic at the TNG–perovskite interface and transport in the device are up to more than 2 times faster than those in the control device or in the recently reported results. With this property, we recorded a power conversion efficiency (PCE) as high as 21.60% (or at the level of 20.84% on average) from the TNG-based PSC with the device area as high as ∼0.17 cm2 using triple cation Cs0.05[MA0.13FA0.87]0.95Pb(I0.87Br0.13)3 perovskites, an improvement as high as 18% from the control device. The TNG with its unique structure and surface chemistry may become a potential platform for the fabrication of a high-performance PSC device via combination with a high-performance perovskite system.

Two-dimensional (2D) perovskite materials are a promising platform to construct high performance photodetectors due to their novel structure, high stability, resistance to ion migration and decent light harvesting ability. However, the detection range of 2D perovskite photodetectors is limited due to their large bandgap. Here, self-trapped states with a lower bandgap were created by introducing Sn into a 2D perovskite ((C6H5C2H4NH3)2PbI4, (PEA)2PbI4). Although previously the excitons in the self-trapped states have been regarded as localized excitons, an obvious photocurrent generated by the dissociation of excitons in self-trapped states has been observed. With this property, the detection range of 2D perovskite photodetectors has been successfully extended. Additionally, the special 2D structure of (PEA)2PbI4 endows the device with high stability and great resistance for ion migration to endure long-term (over 1000 s) consistent work without degradation in performance. This facile doping method for extending the detection range of 2D perovskite photodetectors will greatly broaden their application potential.