Zhu Ziyao, Zhao Bo, He Rui, Chen Huiwen, Gao Sheng, He Yang, Li Yunlong
Shenzhen Institute of Advanced Technology, Chinese Academy of Sciences, Shenzhen 518055, China.
School of Integrated Circuits, Anhui University, Hefei 230039, China.
ACS Appl Mater Interfaces. 2024 Jul 24;16(29):38799-38809. doi: 10.1021/acsami.4c08425. Epub 2024 Jul 14.
The development of perovskite direct X-ray detectors shows potential for advancing medical imaging and industrial inspection precision. To ensure the optimal energy conversion efficiency of X-rays for reducing radiation doses, it is necessary for perovskites with thicknesses reaching hundreds of micrometers or even several millimeters to be utilized. However, the nonlinear current response becomes uncertain with such high thicknesses. For instance, the prevailing theory regarding the rapid trapping and release of charges by shallow-level defects falls short in explaining the nonlinear current response observed in high-quality single-crystal samples. Moreover, a significant nonlinear current response can degrade the detection performance. Here, we elucidate peculiar parasitic and drift capacitance-induced nonlinear current responses in perovskites, which arise from bulk structural deficiencies and interface junction width variation in addition to shallow-level defects. Both theoretical analysis and experimental findings demonstrate the effective suppression of nonlinear current responses by establishing bulk heterojunctions and refining interface junctions. Consequently, we have successfully developed highly linear current-responsive detectors based on polycrystalline MAPbI thick films. Notably, these detectors achieve a record sensitivity of 2.3 × 10 μC·Gy·cm under 100 kV X-ray irradiation with a low bias of 0.1 V/μm, enabling enduring and high-resolution X-ray imaging for high-density objects. Successful fabrication and testing of a 64 × 64-pixel flat-panel prototype detector affirm the widespread applicability of these strategies in rectifying nonlinear current responses in perovskite-based X-ray detectors.
钙钛矿直接X射线探测器的发展显示出提升医学成像和工业检测精度的潜力。为确保X射线的最佳能量转换效率以降低辐射剂量,有必要使用厚度达数百微米甚至几毫米的钙钛矿。然而,对于如此高的厚度,非线性电流响应变得不确定。例如,关于浅能级缺陷对电荷的快速俘获和释放的主流理论,无法解释在高质量单晶样品中观察到的非线性电流响应。此外,显著的非线性电流响应会降低检测性能。在此,我们阐明了钙钛矿中由浅能级缺陷以及体结构缺陷和界面结宽度变化引起的特殊寄生和漂移电容诱导的非线性电流响应。理论分析和实验结果均表明,通过建立体异质结和优化界面结可有效抑制非线性电流响应。因此,我们成功开发了基于多晶MAPbI厚膜的高线性电流响应探测器。值得注意的是,这些探测器在100 kV X射线照射下,以0.1 V/μm的低偏压实现了2.3×10 μC·Gy·cm的创纪录灵敏度,能够对高密度物体进行持久且高分辨率的X射线成像。64×64像素平板原型探测器的成功制造和测试证实了这些策略在纠正基于钙钛矿的X射线探测器中的非线性电流响应方面具有广泛的适用性。