Alvarez Agustin O, Lédée Ferdinand, García-Batlle Marisé, López-Varo Pilar, Gros-Daillon Eric, Guillén Javier Mayén, Verilhac Jean-Marie, Lemercier Thibault, Zaccaro Julien, Marsal Lluis F, Garcia-Belmonte Germà, Almora Osbel
Institute of Advanced Materials, Universitat Jaume I, 12071 Castelló, Spain.
Grenoble Alpes University, CEA, LETI, DOPT, F38000 Grenoble, France.
ACS Phys Chem Au. 2023 May 3;3(4):386-393. doi: 10.1021/acsphyschemau.3c00002. eCollection 2023 Jul 26.
Research on metal halide perovskites as absorbers for X-ray detection is an attractive subject due to the optimal optoelectronic properties of these materials for high-sensitivity applications. However, the contact degradation and the long-term instability of the current limit the performance of the devices, in close causality with the dual electronic-ionic conductivity of these perovskites. Herein, millimeter-thick methylammonium-lead bromide (MAPbBr) single and polycrystalline samples are approached by characterizing their long-term dark current and photocurrent under X-ray incidence. It is shown how both the dark current and the sensitivity of the detectors follow similar trends at short-circuit ( = 0 V) after biasing. By performing drift-diffusion numerical simulations, it is revealed how large ionic-related built-in fields not only produce relaxations to equilibrium lasting up to tens of hours but also continue to affect the charge kinetics under homogeneous low photogeneration rates. Furthermore, a method is suggested for estimating the ionic mobility and concentration by analyzing the initial current at short-circuit and the characteristic diffusion times.
由于金属卤化物钙钛矿材料具有适用于高灵敏度应用的最佳光电特性,因此将其作为X射线检测吸收剂的研究是一个颇具吸引力的课题。然而,目前存在的接触退化和长期不稳定性限制了器件的性能,这与这些钙钛矿的双电子-离子导电性密切相关。在此,通过表征毫米厚的甲基溴化铅(MAPbBr)单晶和多晶样品在X射线照射下的长期暗电流和光电流来进行研究。结果表明,在偏置后短路(= 0 V)时,探测器的暗电流和灵敏度呈现相似的趋势。通过进行漂移-扩散数值模拟,揭示了与离子相关的大内置电场不仅会产生长达数十小时的弛豫至平衡状态,而且在均匀低光生率下仍会继续影响电荷动力学。此外,还提出了一种通过分析短路时的初始电流和特征扩散时间来估算离子迁移率和浓度的方法。