High-performance photodetectors based on zero-dimensional lead-free perovskite thin films
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摘要:
有机-无机杂化非铅钙钛矿因其无生物毒性和环境污染性引起了广泛关注，其中MA3Sb2I9兼具稳定0D结构和非铅的特点，具有应用于稳定、高效光电探测领域的潜力。本文利用MACl后处理的方法来改善反溶剂获得的MA3Sb2I9钙钛矿薄膜的质量，促使MACl与钙钛矿薄膜之间出现Cl-Sb键相互作用，钝化了MA3Sb2I9薄膜表面的I−空位及晶界缺陷。该处理不仅能够有效改善薄膜的表面形貌和结晶性，而且降低了薄膜表面缺陷态密度，提高了载流子提取和传输效率。基于优化薄膜制备的自供电光电探测器件的灵敏度由3.89 × 107 Jones提升至5.72 × 108 Jones，提升了一个数量级；上升/下降时间也由37/76 ms降低到31/37 ms，器件的响应速度也得到了提升。
Abstract:Organic-inorganic hybrid lead-free perovskites have garnered significant attention due to their non-biotoxicity and environmental sustainability. Among these materials, MA3Sb2I9, with its stable zero-dimensional (0D) structure and lead-free nature, shows great promise for stable and efficient photodetection applications. In this study, we employ a MACl post-treatment to enhance the quality of MA3Sb2I9 perovskite thin films fabricated through antisolvent processing. This treatment facilitated the formation of Cl-Sb bond interactions between MACl and the perovskite thin films, effectively passivating the I− vacancies and grain boundary defects on the MA3Sb2I9 thin-film surface. This process not only improve the surface morphology and crystallinity of the thin film but also reduced the defect states density of the surface, thereby enhancing carrier extraction and transport efficiency. Consequently, the sensitivity of self-powered photodetectors based on the optimized thin-film preparation increased from 3.89 × 107 Jones to 5.72 × 108 Jones, representing an improvement by one order of magnitude. Furthermore, the rise and fall times were shortened from 37/76 ms to 31/37 ms, respectively, indicating an enhancement in the response speed of the devices.
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Key words:
- perovskite /
- zero-dimensional /
- lead-free /
- self-powered /
- photodetectors
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图 1 MA3Sb2I9钙钛矿光电探测器的器件结构示意图
Figure 1. Schematic diagram of the device structure of MA3Sb2I9 perovskite photodetector
图 2 不同浓度的 MACl溶液处理后的MA3Sb2I9钙钛矿薄膜的SEM图
Figure 2. SEM images of MA3Sb2I9 perovskite thin films treated with different concentrations of MACl solution
图 3 MACl处理前后的MA3Sb2I9钙钛矿薄膜的（a）UV-vis光谱（b）XRD图
Figure 3. (a) UV-vis spectra, (b) XRD patterns of the MA3Sb2I9 perovskite thin films before and after the MACl treated
图 4 不同浓度MACl处理前后的钙钛矿薄膜XPS（a）全谱，高分辨率的（b）Cl 2p（c）Sb 3d（d）I 3d图谱
Figure 4. XPS measurement of the (a) full spectrum, high-resolution spectrum of (b) Cl 2p (c) Sb 3d (d) I 3d of perovskite thin films before and after MACl treatment with different concentrations
图 5 不同浓度MACl处理前后的MA3Sb2I9钙钛矿薄膜的（a）PL谱（b）TRPL谱
Figure 5. (a) Steady-state PL, (b) TRPL spectrum of MA3Sb2I9 perovskite thin films before and after MACl treatment with different concentrations
图 6 MACl处理前后MA3Sb2I9钙钛矿薄膜的水接触角图
Figure 6. Water contact angle of MA3Sb2I9 perovskite thin films before and after MACl treatment
图 7 MA3Sb2I9钙钛矿光电探测器：（a）经不同浓度MACl后处理的暗态I-V曲线，（b）未处理和最优条件下的光、暗态I-V曲线
Figure 7. (a) Dark I-V curves of MA3Sb2I9 perovskite photodetectors treated with different concentrations of MACl, (b) light and dark I-V curves of untreated and optimal conditions
图 8 MA3Sb2I9钙钛矿光电探测器的（a）Jsc统计图，（b）EQE，（c）R，（d）D*
Figure 8. (a) Jsc distribution, (b) R, (c) EQE, (d) D* of the MA3Sb2I9 perovskite photodetector
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