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With the surge in perovskite research, practical features for future applications are desired to be secured, but the reliability of the materials and the use of hazardous Pb are longstanding problems. Here, an air‐stable Cs2SnI6 (CSI) is prepared via diluted hydriodic acid solvent‐based precursor optimization during scalable hydrothermal growth. Materials characterization is performed using various elemental peak analyses and crystallographic identification. The resulting CSI exhibits long‐term operating stability over 6 months, i) at elevated temperatures, ii) in ambient air, and iii) under light illumination from UV to near‐infrared. More importantly, to demonstrate an intriguing class of applications up to system level, physically detachable CSI photodetector arrays (PD‐arrays), integrated with micro‐light‐emitting‐diodes (μ‐LEDs) arrays, are successfully fabricated. In addition, 3 × 3 flexible CSI PDs are fully operational, even in air, and their spatial uniformity in pixels is quantitatively evaluated. The charge‐transport mechanisms of the CSI PDs under light and elevated temperature are assessed via temperature‐dependent characterization from 148 to 373 K, implying the involvement of 3D variable‐range hopping. Multicycle evaluation of the CSI PD‐arrays confirms their operational stability in AC and DC modes, demonstrating this platform's potential benefit for wireless optical interconnection in advanced Si technology.

Contact layers play an important role in thin film solar cells, but new material development and optimization of its thickness is usually a long and tedious process. A high-throughput experimental approach has been used to accelerate the rate of research in photovoltaic (PV) light absorbers and transparent conductive electrodes, however the combinatorial research on contact layers is less common. Here, we report on the chemical bath deposition (CBD) of CdS thin films by combinatorial dip coating technique and apply these contact layers to Cu(In,Ga)Se2 (CIGSe) and Cu2ZnSnSe4 (CZTSe) light absorbers in PV devices. Combinatorial thickness steps of CdS thin films were achieved by removal of the substrate from the chemical bath, at regular intervals of time, and in equal distance increments. The trends in the photoconversion efficiency and in the spectral response of the PV devices as a function of thickness of CdS contacts were explained with the help of optical and morphological characterization of the CdS thin films. The maximum PV efficiency achieved for the combinatorial dip-coating CBD was similar to that for the PV devices processed using conventional CBD. The results of this study lead to the conclusion that combinatorial dip-coating can be used to accelerate the optimization of PV device performance of CdS and other candidate contact layers for a wide range of emerging absorbers.