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基于氘代卤化物钙钛矿单晶的低降解高灵敏度X射线探测器。

High Sensitivity X-Ray Detectors with Low Degradation Based on Deuterated Halide Perovskite Single Crystals.

作者信息

Liu Lishan, Xu Mingxia, Xu Xinguang, Tao Xutang, Gao Zeliang

机构信息

State Key Laboratory of Crystal Materials, Shandong University, Jinan, Shandong, 250100, China.

出版信息

Adv Mater. 2024 Nov;36(44):e2406443. doi: 10.1002/adma.202406443. Epub 2024 Sep 16.

Abstract

Methylammonium lead single crystal (MAPbI SC) possesses superior optoelectronic properties and low manufacturing cost, making it an ideal candidate for X-ray detection. However, the ionic migration of the perovskites usually leads to instability, dark current drift, and hysteresis of the detector, limiting their applications in well-established technologies. Here, a series of X-ray detectors of MAPbI SCs are reported with different degrees of deuteration (DMAPbI, x = 0, 0.15, 0.75, 0.99). By controlling the content of deuterium (D) in organic cations, the sensitivity, detection limits, ion migration, and resistivity of the detector can be controlled, thereby improving its performance. Due to stronger hydrogen bonds (N─D···I), the ion activation energy significantly increases to 886 meV. Consequently, the DMAPbI SC detector shows more than five-fold enhancement, achieving a record-high mobility-lifetime (µτ) product of 5.39 × 10 cm V, with an ultrahigh sensitivity of 2.18 × 10 µC Gy cm under 120 keV hard X-ray and a low detection limit of 4.8 nGy s, as well as long-term stability. The study provides a straightforward strategy for constructing ultrasensitive X-ray detection and imaging systems based on perovskite SCs.

摘要

甲脒铅单晶(MAPbI SC)具有优异的光电性能和较低的制造成本,使其成为X射线检测的理想候选材料。然而,钙钛矿的离子迁移通常会导致探测器的不稳定性、暗电流漂移和滞后现象,限制了它们在成熟技术中的应用。在此,报道了一系列不同氘化程度(DMAPbI,x = 0、0.15、0.75、0.99)的MAPbI SC X射线探测器。通过控制有机阳离子中氘(D)的含量,可以控制探测器的灵敏度、检测限、离子迁移和电阻率,从而提高其性能。由于更强的氢键(N─D···I),离子活化能显著增加至886 meV。因此,DMAPbI SC探测器显示出超过五倍的增强,实现了创纪录的高迁移率-寿命(µτ)乘积5.39 × 10 cm V,在120 keV硬X射线下具有2.18 × 10 µC Gy cm的超高灵敏度和4.8 nGy s的低检测限,以及长期稳定性。该研究为构建基于钙钛矿SC的超灵敏X射线检测和成像系统提供了一种直接的策略。

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