铅卤钙钛矿的光稳定性研究进展

楼浩然; 叶志镇; 何海平

doi:10.7498/aps.68.20190324

摘要

铅卤钙钛矿可实现溶液法制备且具有诸多优异的光电特性, 在高效太阳能电池、发光二极管、激光、光探测器等光电子领域具有广阔的应用前景. 但是铅卤钙钛矿在光辐照下存在不稳定问题, 严重影响其相关光电器件的寿命和性能稳定性. 因此, 铅卤钙钛矿在持续光照下的不稳定性现象及其机理正受到越来越多的关注. 本文综述了铅卤钙钛矿在持续光照下的四类主要不稳定现象, 即光修复现象、光解现象、光致相分离现象以及光致相变现象, 并介绍目前已提出的相关机理, 分别从缺陷态、离子迁移、热力学原理、化学键等角度来解释其光照不稳定性. 最后, 本文简要讨论了钙钛矿中光稳定性研究的复杂性及未来需要解决的问题.

关键词:

铅卤钙钛矿 /
光稳定性 /
机理

Abstract

Lead halide perovskites, which can be grown by solution process, are very suitable for various optoelectronic applications, such as in solar cells, light-emitting diodes, lasers and photo-detectors, due to their outstanding electrical and optical properties. However, lead halide perovskites are unstable under continuous light illumination, which severely degrades the performance and lifetime of optoelectronic devices based on them. Therefore, the photo-stability of perovskites and the mechanisms have received more and more attention. In this article we review the main phenomena in perovskites, induced by continuous light illumination, namely photo curing, photo dissociation, photo-induced phase separation, and photo-induced phase transition. The proposed mechanisms for the instability from the perspectives of defect states, ion migration, thermodynamics and chemical bonds, respectively, are also introduced. Finally, the complexity presented in the studying of photo-stability, and the issues should be addressed in the future are also briefly discussed.

Keywords:

作者及机构信息

浙江大学材料科学与工程学院, 硅材料国家重点实验室, 杭州　310027

通信作者: 何海平, hphe@zju.edu.cn

基金项目: 国家自然科学基金(批准号: 51772271)资助的课题.

Authors and contacts

State Key Laboratory of Silicon Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou 310027, China

Corresponding author: He Hai-Ping, hphe@zju.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant No. 51772271).

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施引文献

图 1 铅卤钙钛矿ABX₃的结构示意图^[1]

Fig. 1. Structure of lead halide perovskites^[1].

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图 2 铅卤钙钛矿及其太阳能电池在持续光照下发生光修复现象时的性能变化　(a) CH₃NH₃PbI₃薄膜在持续光照下的时间分辨PL衰减随光照时间的变化^[57]; (b) CH₃NH₃PbI₃薄膜在持续光照下以及不同温度下的PL强度随光照时间的变化^[57]; (c) 铅卤钙钛矿太阳能电池ITO/PEDOT:PSS/CH₃NH₃PbI_3–xCl_x/PCBM/Al在持续光照下的J-V曲线变化^[62]; (d) 铅卤钙钛矿太阳能电池ITO/PEDOT:PSS/CH₃NH₃PbI_3–xCl_x/PCBM/Al在持续光照下的光电转化效率的变化曲线^[62]

Fig. 2. Performance changes of lead halide perovskite and its solar cells under continuous illunination: (a) A series of time-resolved PL decays from CH₃NH₃PbI₃ films measured over time under continuous illumination^[57]; (b) the normalized PL intensity of CH₃NH₃PbI₃ films measured over time under continuous illumination at different temperatures^[57]; (c) the J-V characteristics of lead halide perovskite solar cell with the architecture of ITO/PEDOT:PSS/CH₃NH₃PbI_3–xCl_x/PCBM/Al under continuous illumination^[62]; (d) the reversibility of power conversion efficiency of lead halide perovskite solar cell with the architecture of ITO/PEDOT:PSS/CH₃NH₃PbI_3–xCl_x/PCBM/Al under continuous illumination^[62].

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图 3 CH₃NH₃PbI₃薄膜发生光修复现象的机理^[57]　(a) 在发光较弱的晶粒中分布有高浓度的缺陷态以及过量的碘离子; (b) CH₃NH₃PbI₃薄膜经过光照后, 电子迅速填充缺陷, 产生电场, 造成碘离子从照射区域开始迁移, 填充空位; (c)照射区域中的缺陷态密度和碘离子浓度降低, 薄膜最终达到稳定的状态; (d) 当移除光照后, 碘离子存在浓度梯度, 驱使其扩散回弱发光区域, 直至达到新的碘离子浓度平衡

Fig. 3. Mechanism of photo curing in CH₃NH₃PbI₃ film^[57]: (a) Iodide in a "dark spot" is initially high with a corresponding excess of trap density; (b) electrons quickly fill traps under illumination, inducing an electric field that results in iodide to migrate away from the illuminated region and fill vacancies; (c) the fill will reaches a stabilized state, with the reduction of the density of the traps and the concentration of the iodide in illuminated region; (d) when the illumination is removed, there may be a concentration gradients driving some iodides in to the dark spot and the film will reaches a new equilibrium with a net redistributed iodide profile.

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图 4 (a) 传统旋涂法制备的CH₃NH₃PbI₃薄膜在激发密度0.2和0.65 W/cm²下的光致发光强度随时间的变化; (b) 气体辅助溶液工程技术制备的CH₃NH₃PbI₃薄膜在激发密度0.90, 1.55和2.00 W/cm²下的光致发光强度随时间的变化; (c) 传统旋涂法以及气体辅助溶液工程技术制备的CH₃NH₃PbI₃薄膜的光致发光谱和吸收光谱^[49]

Fig. 4. (a) PL intensities over time of CH₃NH₃PbI₃ film fabricated by conventional spin coating under laser excitations at 0.2 and 0.65 W/cm²; (b) PL intensities over time of CH₃NH₃PbI₃ film fabricated by gas-assisted solution process technique under laser excitations at 0.9, 1.55 and 2.00 W/cm²; (c) absorption and PL spectra of samples fabricated conventional spin coating and gas-assisted solution process technique^[49].

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图 5 (a) CH₃NH₃PbI₃薄膜在黑暗-光照-黑暗循环中的光致发光强度随时间的变化; (b) CH₃NH₃PbI₃薄膜的光致发光谱随黑暗或光照下放置时间的变化; (c) CH₃NH₃PbI₃薄膜的实验中和理论上的拉曼光谱以及CH₃NH₃PbI₃薄膜在黑暗环境和光照20, 40和60 min后的拉曼光谱^[58]

Fig. 5. (a) PL measurements performed throughout a dark-light-dark cycle, showing the effect of white-light illumination on the PL intensity of the CH₃NH₃PbI₃ film; (b) a graph showing six PL measurements points from the dark-light-dark cycles at different times; (c) a graph showing Experimental (taken in the dark) and theoretical Raman spectra of a CH₃NH₃PbI₃ film as well as the Raman spectra of the same film taken in the dark and following illumination for 20, 40 and 60 min^[58]

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图 6 (a) 铅卤钙钛矿太阳能电池ITO/PEDOT:PSS/MAPbI₃/PCBM/Al在持续光照下的光电转化效率的变化趋势, 其中工作条件A对应于J = 0, V = V_oc; 工作条件B对应于J = J_sc, V = 0; (b) 铅卤钙钛矿材料发生可逆光解现象的机理^[76]

Fig. 6. (a) Time evolution of power conversion efficiency of lead halide perovskite solar cell with the architecture of ITO/PEDOT:PSS/MAPbI₃/PCBM/Al under constant 1-Sun illumination. The device is stressed at point A (red circles, J = 0, V = V_oc) or point B (blue squares, J = J_sc, V = 0); (b) schematics of the photocurrent degradation and self-healing mechanism^[76].

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图 7 (a) 铅卤钙钛矿太阳能电池FTO/TiO₂/mp-TiO₂/(FAPbI₃)_x(MAPbBr₃)_y/spiro-OMeTAD/Au在滤过紫外光后的LED灯光持续照射下的最大功率输出的变化趋势; (b) 钙钛矿层中的离子分布的变化趋势^[59]

Fig. 7. (a) Maximum power output tracking for 3 identically prepared perovskite solar cells (device A, B and C), with the architecture of FTO/TiO₂/mp-TiO₂/(FAPbI₃)_x(MAPbBr₃)_y/spiro-OMeTAD/Au, measured under UV-filtered 1-Sun LED illumination. Experimental data were fitted to an exponential decay (single or double). (b) Schematics of the evolution of ion distribution within the perovskite layer^[59].

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图 8 (a) CH₃NH₃Pb(Br_0.6I_0.4)₃在激发密度50 mW/cm²下光照5 min前(黑线)和后(红线)的XRD图像, 其中虚线分别为CH₃NH₃Pb(Br_0.2I_0.8)₃和CH₃NH₃Pb(Br_0.7I_0.3)₃的XRD图像^[47]; (b) CH₃NH₃Pb(Br_0.4I_0.6)₃在激发密度为15 mW/cm²的457 nm激光持续照射下的光致发光谱的变化趋势^[47]; (c) CH₃NH₃Pb(Br_0.9I_0.1)₃在激发密度为50 mW/cm²的405 nm激光持续照射下的阴极发光图像随时间的变化^[86]; (d) CH₃NH₃Pb(Br_1–xI_x)₃在光照下发生光致相分解现象的机理^[46]

Fig. 8. (a) The XRD peak of CH₃NH₃Pb(Br_0.6I_0.4)₃ film before (black) and after (red) white-light soaking for 5 minutes 50 mW/cm². XRD patterns of CH₃NH₃Pb(Br_0.2I_0.8)₃ and CH₃NH₃Pb(Br_0.7I_0.3)₃ films (dashed brown) are included for comparison^[47]; (b) photoluminescence spectra of CH₃NH₃Pb(Br_0.4I_0.6)₃ film over 45 s in 5 s increments under 457 nm, 15 mW/cm² at 300 K^[47]; (c) a series of cathodo luminescence image after light soaking under a 405 nm LED at 50 mW/cm²^[86]; (d) the schematic of two-step mechanism for light-induced phase separation^[46].

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图 9 铅卤钙钛矿在持续光照下发生的主要四种不稳定现象　(a) 碘间隙离子/碘空位缺陷对的消除引起光修复现象; (b) 碘空位与阳离子空位的迁移引起光解现象; (c) 亥姆霍兹自由能最小化促使铅卤钙钛矿内部的卤素离子从无序排列向有序排列, 引起光致相分离现象; (d) 光生载流子迁移率差异产生电位差, 造成PBI₆^4–六面体扭力方向的改变, 引起光致相变现象

Fig. 9. Main four kinds of instability of lead halide perovskites under continuous illumination: (a) Photo-curing induced by the elimination of iodine interstitial ions/iodine vacancies; (b) photo dissociation induced by the migration of iodine vacancies and cation vacancies; (c) phase separation induced by the minimization of Helmholtz free energy; (d) phase transition induced by the difference in the mobility of electrons and holes.

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