High-performance photodetectors based on zero-dimensional lead-free perovskite thin films
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摘要:
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: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 the efficiency of carrier extraction and transport. 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 by MACl solution with different concentrations
图 3 MACl处理前后的MA3Sb2I9钙钛矿薄膜的（a）UV-vis光谱及（b）XRD图
Figure 3. (a) UV-vis spectra and (b) XRD patterns of the MA3Sb2I9 perovskite thin films before and after the MACl treatment
图 4 不同浓度MACl处理前后的钙钛矿薄膜（a）XPS全谱及高分辨率的（b）Cl 2p（c）Sb 3d（d）I 3d图谱
Figure 4. (a) XPS measurement 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钙钛矿光电探测器处理结果。（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-state I-V curves of MA3Sb2I9 perovskite photodetectors treated with MACl of different concentrations, (b) light and dark-state I-V curves of under 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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