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摘要

钙钛矿薄膜的气相制备是一种极具潜力的工业化生产工艺, 但薄膜的质量控制目前远落后于溶液制备法. 本文通过建立PbI ₂薄膜向钙钛矿薄膜完全转化过程中反应时间、晶粒尺寸与温度的关系, 实现了薄膜的质量优化及大面积钙钛矿薄膜的制备, 将薄膜的平均晶粒粒径从0.42 ${\text{μm}}$ 优化到0.81 ${\text{μm}}$ . 基于空间电荷限制电流模型对缺陷密度的研究显示, 钙钛矿薄膜的缺陷密度由5.90 × 10 ¹⁶cm ^–3降低到2.66 × 10 ¹⁶cm ^–3. 光伏器件(FTO/TiO ₂/C ₆₀/MAPbI ₃/spiro-OMeTAD/Au结构)测试显示, 面积为0.045 cm ²器件的平均光电转换效率从14.00%提升到17.42%, 最佳光电转换效率达到17.80%, 迟滞因子减小至4.04%. 同时, 基于180 ℃制备的1 cm ²器件的光电转换效率达到13.17%.

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Abstract

Organometal halide perovskite is one of the most promising materials for high efficient thin-film solar cell. Solution fabrication process shows that the recorded power conversion efficiency (PCE) is 23.7%, however, large scale fabrication suffers the inevitable toxic solvent, preventing it from implementing the green commercialization. As one of the matured large-scale fabrication techniques, the vapor deposition is recently found to promise the green fabrication of perovskite thin film without toxic solvent. However, the PCE based on vapor deposition is considerably lower than that based on solution fabrication because of ineffective regulation methods of the perovskite films. So, there is intensive requirement for optimizing the growth of perovskite in vapor deposition for improving PCE, especially, developing a kind of quality regulation method of the perovskite films. In this study, we provide a method of adjusting grain size in vapor deposition method. The grain size optimization of MAPbI ₃films is realized by simply modulating the reaction temperature between PbI ₂films and MAI vapor. We set the reaction temperature to be 140 ℃, 160 ℃, 180 ℃ and 200 ℃ separately and establish the relationship between reaction time and grain size during the complete conversion of PbI ₂film into MAPbI ₃film. We find that the average grain size of the film increases first with growth temperature increasing from 140 ℃ to 180 ℃ and then decrease at 200 ℃, giving an average grain size of 0.81 ${\text{μm}}$ and a largest grain size of about 2 ${\text{μm}}$ at 180 ℃. The defect density of perovskite film is deduced from the space charge limited current model, showing that it decreases from 5.90 × 10 ¹⁶cm ^–3at 140 ℃ to 2.66 × 10 ¹⁶cm ^–3at 180 ℃. Photovoltaic devices with structure FTO/TiO ₂/C ₆₀/MAPbI ₃/spiro-OMeTAD/Au are fabricated to demonstrate the performance. It is found that the devices with an active area of 0.045 cm ²show that with the increase of grain size, the average PCE increases from 14.00% to 17.42%, and the best device shows that its PCE is 17.80% with 4.04% hysteresis index. To show the possibility of scaling up, we fabricate a uniform perovskite thin film with an area of about 72 cm ², and a device with an active area of 1 cm ², which gives a PCE of 13.17% in reverse scan. In summary, our research provides a method of regulating the grain size for the vapor deposition, which can improve device performance by reducing the trap density in perovskite film for suppressing the carrier recombination in grain boundary. Meanwhile, we prepare high performance devices and large area thin films, showing their potential in large area device fabrication and applications.

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作者及机构信息

通信作者:谢伟广,wgxie@email.jnu.edu.cn; 刘彭义,tlpy@jnu.edu.cn

基金项目:国家自然科学基金(批准号: 61674070, 11574119, 11804117)和中央高校基本科研业务费专项资金资助(暨南大学科研培养与创新基金)(批准号: 21618313) 资助的课题.

Authors and contacts

Corresponding author:Xie Wei-Guang,wgxie@email.jnu.edu.cn; Liu Peng-Yi,tlpy@jnu.edu.cn

Funds:Project supported by the National Natural Science Foundation of China (Grant Nos. 61674070, 11574119, 11804117) and the Fundamental Research Funds for the Central Universities, China (Grants No. 21618313).

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参考文献

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施引文献

下载: 全尺寸图片幻灯片

Sythesis temperature	J_sc/mA·cm^-2	V_oc/V	FF/%	Champion PCE/%	Average PCE/%
140	22.04	0.99	66.31	14.47	14.00
160	22.25	1	70.51	15.69	14.93
180	23.47	1.02	74.35	17.80	17.42
200	22.75	1.03	70.88	16.61	16.13

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