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.
| Original language | English |
|---|---|
| Article number | 2106295 |
| Journal | Advanced Functional Materials |
| Volume | 31 |
| Issue number | 50 |
| DOIs | |
| Publication status | Published - 2021 |
| Publication type | A1 Journal article-refereed |
Funding
J.M. and V.P. contributed equally to this work. J.M. is thankful to Yueheng Peng, Fengzhu Li, and Kai Xia for training. V.P. is thankful to Dr. Nicola Gasparini for helpful discussions. V.P. acknowledges financial support from the National Natural Science Foundation of China (61805166), the Collaborative Innovation Center of Suzhou Nano Science and Technology, the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD), the 111 Project, and the Joint International Research Laboratory of Carbon‐Based Functional Materials and Devices. M.L. thanks the Finnish Cultural Foundation (00210670) for funding. P.V. acknowledges Jane and Aatos Erkko foundation (project ASPIRE) for financial support and the Academy of Finland Flagship Programme, Photonics Research and Innovation (PREIN), Decision No. 320165.
Keywords
- antimony-based perovskite derivatives
- lead-free perovskite-inspired materials
- linear dynamic range
- self-powered photodetectors
- structural dimensionality
Publication forum classification
- Publication forum level 3
ASJC Scopus subject areas
- General Chemistry
- General Materials Science
- Condensed Matter Physics
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