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The vast chemical space of emerging semiconductors, like metal halide perovskites, and their varied requirements for semiconductor applications have rendered trial-and-error environmentally unsustainable. In this work, we demonstrate RoboMapper, a materials acceleration platform (MAP), that achieves 10-fold research acceleration by formulating and palletizing semiconductors on a chip, thereby allowing high-throughput (HT) measurements to generate quantitative structure-property relationships (QSPRs) considerably more efficiently and sustainably. We leverage the RoboMapper to construct QSPR maps for the mixed ion FA 1-y Cs y Pb(I 1-x Br x ) 3 halide perovskite in terms of structure, bandgap, and photostability with respect to its composition. We identify wide-bandgap alloys suitable for perovskite-Si hybrid tandem solar cells exhibiting a pure cubic perovskite phase with favorable defect chemistry while achieving superior stability at the target bandgap of 1.7 eV. RoboMapper’s palletization strategy reduces environmental impacts of data generation in materials research by more than an order of magnitude, paving the way for sustainable data-driven materials research. 

Reduced open-voltage deficit and enhanced light absorption enable bifacial tandem device with equivalent efficiency of 29.3% 

Abstract High‐performance tin‐lead perovskite solar cells (PSCs) are needed for all‐perovskite‐tandem solar cells. However, iodide related fast photodegradation severely limits the operational stability of Sn‐Pb perovskites despite the demonstrated high efficiency and thermal stability. Herein, this work employs an alkylammonium pseudo‐halogen additive to enhance the power conversion efficiency (PCE) and photostability of methylammonium (MA)‐free, Sn‐Pb PSCs. Density functional theory (DFT) calculations reveal that the pseudo‐halogen tetrafluoroborate (BF₄⁻) has strong binding capacity with metal ions (Sn²⁺/Pb²⁺) in the Sn‐Pb perovskite lattice, which lowers iodine vacancy formation. Upon combining BF₄⁻with an octylammonium (OA⁺) cation, the PCE of the device with a built‐in light‐scattering layer is boosted to 23.7%, which represents a new record for Sn‐Pb PSCs. The improved efficiency benefits from the suppressed defect density. Under continuous 1 sun illumination, the OABF₄embodied PSCs show slower generation of interstitial iodides and iodine, which greatly improves the device photostability under open‐circuit condition. Moreover, the device based on OABF₄retains 88% of the initial PCE for 1000 h under the maximum‐power‐point tracking (MPPT) without cooling.