全无机钙钛矿X射线光导体多晶厚膜制备工艺研究

X射线探测器在医疗影像、工业检测、安全检查和材料分析等领域被广泛应用。近年来，金属卤化物钙钛矿由于具有高X射线吸收系数、高载流子迁移率寿命积、高电阻率和可低成本制备等优点，成为下一代X射线光导体（X-ray photoconductor）的研究热点。其中，有机-无机杂化钙钛矿突出的光电性能赋予其出色的X射线响应，但由于杂化钙钛矿中有机阳离子的吸湿性和挥发性，导致其在湿气、氧气、紫外线和加热等环境下易分解。不含有机成分的全无机钙钛矿拥有更高的光热稳定性和X射线吸收系数，有望突破钙钛矿材料在X射线探测领域的应用瓶颈，然而，目前全无机钙钛矿探测器的性能仍远低于有机-无机杂化钙钛矿。

因此，本文围绕以上问题，基于全无机铯铅溴（CsPbBr₃）钙钛矿，提出稀土氧化物复合结构调控X射线光电导策略，获得媲美有机-无机杂化钙钛矿的器件性能，从而推动高性能全无机卤化物钙钛矿X射线探测器的发展；进一步以Ag、Bi取代Pb合成非铅钙钛矿铯银铋溴（Cs₂AgBiBr₆），探索环境友好型全无机钙钛矿X射线探测器的应用潜力。主要内容如下：

本文选取了无机卤化物钙钛矿CsPbBr₃作为X射线光导体材料，通过构建以稀土氧化物氧化钇（Y₂O₃）为骨架的二元高稳定无机复合体系提升CsPbBr₃的稳定性的同时降低CsPbBr₃的缺陷密度，提升载流子收集效率，调控其X射线光电导性能，通过冷压的方式制备X射线光导体厚膜，最终制备的X射线探测器的灵敏度高达2.5×10⁷ μC·Gy_air^-1·cm^-2，检测限低至3.3 nGy_air·s^-1。

同时，本文选取了全无机非铅的双钙钛矿Cs₂AgBiBr₆作为X射线光导体材料。通过浆料刮涂的方法制备Cs₂AgBiBr₆厚膜，以苯乙基乙酸铵（PEAAc）钝化晶界，减少厚膜内部缺陷密度，降低外界环境中水氧的影响，同时提升厚膜的电阻率及离子迁移活化能，降低暗电流密度及基线漂移，构建的X射线探测器暗电流漂移低至8.5×10^-9 nA·cm^-1·s^-1·V^-1。

总之，本工作为提高全无机卤化物钙钛矿X射线探测器的性能提供了一种有前景的方法，证明了CsPbBr₃钙钛矿和非铅Cs₂AgBiBr₆钙钛矿作为X射线光导体的潜力。

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