Two-Dimensional Antimony-Based Perovskite-Inspired Materials for High-Performance Self-Powered Photodetectors

Abstract

The ongoing Internet of Things revolution has led to strong demand for low-cost, ubiquitous light sensing based on easy-to-fabricate, self-powered photodetectors. While solution-processable lead-halide perovskites have raised significant hopes in this regard, toxicity concerns have prompted the search for safer, lead-free perovskite-inspired materials (PIMs) with similar optoelectronic potential. Antimony- and bismuth-based PIMs are found particularly promising; however, their self-powered photodetector performance to date has lagged behind the lead-based counterparts. Aiming to realize the full potential of antimony-based PIMs, this study examines, for the first time, the impact of their structural dimensionality on their self-powered photodetection capabilities, with a focus on 2D Cs3Sb2I9−xClx and Rb3Sb2I9 and 0D Cs3Sb2I9. The 2D absorbers deliver cutting-edge self-powered photodetector performance, with a more-than-tenfold increase in external quantum efficiency (up to 55%), speed of response (>5 kHz), and linear dynamic range (>four orders of magnitude) compared to prior self-powered A3M2X9 implementations (A+: monovalent cation; M3+: Sb3+/Bi3+; X−: halide anion). Detailed characterization reveals that such a performance boost originates from the superior carrier lifetimes and reduced exciton self-trapping enabled by the 2D structure. By delivering cutting-edge performance and mechanistic insight, this study represents an important step in lead-free perovskite-inspired optoelectronics toward self-powered, ubiquitous light sensing.