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Revisiting Sub-Band Gap Emission Mechanism in 2D Halide Perovskites: The Role of Defect States

激子 光致发光 化学 载流子 光谱学 密度泛函理论 带隙 X射线光电子能谱 光电子学 自发辐射 化学物理 分子物理学 凝聚态物理 材料科学 计算化学 物理 光学 量子力学 核磁共振 激光器
作者
Igal Levine,Dorothee Menzel,Artem Musiienko,Rowan W. MacQueen,N Romano,Manuel Vásquez-Montoya,Eva Unger,Carlos Mora Perez,Aaron Forde,Amanda J. Neukirch,Lars Korte,Thomas Dittrich
出处
期刊:Journal of the American Chemical Society [American Chemical Society]
卷期号:146 (33): 23437-23448 被引量:5
标识
DOI:10.1021/jacs.4c06621
摘要

Understanding the sub-band gap luminescence in Ruddlesden–Popper 2D metal halide hybrid perovskites (2D HaPs) is essential for efficient charge injection and collection in optoelectronic devices. Still, its origins are still under debate with respect to the role of self-trapped excitons or radiative recombination via defect states. In this study, we characterized charge separation, recombination, and transport in single crystals, exfoliated layers, and polycrystalline thin films of butylammonium lead iodide (BA2PbI4), one of the most prominent 2D HaPs. We combined complementary defect- and exciton-sensitive methods such as photoluminescence (PL) spectroscopy, modulated and time-resolved surface photovoltage (SPV) spectroscopy, constant final state photoelectron yield spectroscopy (CFSYS), and constant light-induced magneto transport (CLIMAT), to demonstrate striking differences between charge separation induced by dissociation of excitons and by excitation of mobile charge carriers from defect states. Our results suggest that the broad sub-band gap emission in BA2PbI4 and other 2D HaPs is caused by radiative recombination via defect states (shallow as well as midgap states) rather than self-trapped excitons. Density functional theory (DFT) results show that common defects can readily occur and produce an energetic profile that agrees well with the experimental results. The DFT results suggest that the formation of iodine interstitials is the initial process leading to degradation, responsible for the emergence of midgap states, and that defect engineering will play a key role in enhancing the optoelectronic properties of 2D HaPs in the future.
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