Antimony-bismuth alloying: the key to a major boost in the efficiency of lead-free perovskite-inspired indoor photovoltaics

Perovskite-inspired Cu2AgBiI6 (CABI) absorber has recently gained increased popularity due to its low toxicity, intrinsic air stability, and wide bandgap ≈ 2 eV, which makes it ideal for indoor photovoltaics (IPVs). However, the considerable presence of both intrinsic and surface defects is responsible of the still modest indoor power conversion efficiency (PCE(i)) of CABI- based IPVs, with the short-circuit current density (JSC) being nearly half of the theoretical limit. Herein, we introduce antimony (III) (Sb3+) into the octahedral lattice sites of CABI structure, leading to CABI-Sb with substantially larger crystalline domains than CABI. The alloying of Sb3+ with bismuth (III) (Bi3+) induces changes in the local structural symmetry, in turn causing a remarkably increased formation energy of intrinsic defects. This accounts for the overall reduced defect density in CABI-Sb. CABI-Sb IPVs feature an outstanding PCE(i) of nearly 10% (9.53%) at 1000 lux, which represents an almost double PCE(i) compared to that of CABI devices (5.52%) mainly due to an improvement in JSC. This work will promote future compositional design studies to reduce the intrinsic defect tolerance of next-generation wide- bandgap absorbers for high-performance and stable IPVs.