Liu Yongtao, Borodinov Nikolay, Collins Liam, Ahmadi Mahshid, Kalinin Sergei V, Ovchinnikova Olga S, Ievlev Anton V
Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37830, United States.
Department of Materials Science and Engineering, University of Tennessee, Knoxville, Tennessee 37996, United States.
ACS Nano. 2021 May 25;15(5):9017-9026. doi: 10.1021/acsnano.1c02097. Epub 2021 May 6.
Ion migration is one of the most debated mechanisms and credited with multiple observed phenomena and performance in metal halide perovskites (MHPs) semiconductor devices. However, to date, the migration of ions and their effects on MHPs are not still fully understood, largely due to a lack of direct observations of temporal ion migration. In this work, using direct observation of ion migration , we observe the hysteretic migration behavior of intrinsic ions (, CHNH and I) as well as reveal the migration behavior of CHNH decomposition ions. We find that CHNH decomposition products can be affected by light and accumulate at the interfaces under bias. These MHP decomposition products are tightly related to the device performance and stability. Complementary results of time-resolved Kelvin probe force microscopy (tr-KPFM) demonstrate a correlation between dynamics of these interfacial ions and charge carriers. Overall, we find that there are a number of mobile ions including CHNH decomposition products in MHPs that need to be taken into account when measuring MHP device responses (, charge dynamics) and should be considered in future optimization studies of MHP semiconductor devices.
离子迁移是金属卤化物钙钛矿(MHPs)半导体器件中最具争议的机制之一,与多种观察到的现象和性能有关。然而,迄今为止,离子的迁移及其对MHPs的影响仍未被完全理解,这主要是由于缺乏对离子迁移时间的直接观察。在这项工作中,通过直接观察离子迁移,我们观察到了本征离子(、CHNH和I)的滞后迁移行为,并揭示了CHNH分解离子的迁移行为。我们发现,CHNH分解产物会受到光的影响,并在偏压下在界面处积累。这些MHP分解产物与器件性能和稳定性密切相关。时间分辨开尔文探针力显微镜(tr-KPFM)的补充结果表明,这些界面离子的动力学与电荷载流子之间存在相关性。总体而言,我们发现在测量MHP器件响应(如电荷动力学)时,需要考虑MHPs中包括CHNH分解产物在内的大量可移动离子,并且在未来MHP半导体器件的优化研究中也应予以考虑。