Eutectic Urea Phosphate Suppresses Phase Segregation in Wide‐Bandgap Photovoltaic Perovskites

ABSTRACT Compositional segregation resulting from non‐uniform crystallization remains a critical bottleneck limiting the performance of wide‐bandgap (WBG) mixed‐halide perovskite photovoltaics. Herein, we report a halide‐specific coordination strategy by employing a eutectic molecule to stop the phase segregation in WBG perovskites. Owing to the differential affinity of stronger for bromine‐based octahedra than iodine‐based ones, the urea phosphate molecule acts as a molecular pacemaker synchronizing the crystallization of disparate perovskite phases. This strategy successfully eliminates vertical and lateral phase segregation within the films, leading to a substantial reduction in non‐radiative recombination and charge transport losses. Consequently, the champion perovskite photovoltaic devices present a power conversion efficiency (PCE) of 22.27% under AM 1.5G illumination and a promising indoor PCE of 42.64% under 1000 lux. The finding offers a robust paradigm to fabricate high‐quality WBG photovoltaic perovskites for indoor energy harvesting in the Internet of Things.