Point defects in metal halide perovskites play a critical role in determining their properties and optoelectronic performance; however, many open questions remain unanswered. In this work, we apply impedance spectroscopy and deep-level transient spectroscopy to characterize the ionic defect landscape in methylammonium lead triiodide (MAPbI3) perovskites in which defects were purposely introduced by fractionally changing the precursor stoichiometry. Our results highlight the profound influence of defects on the electronic landscape, exemplified by their impact on the device built-in potential, and consequently, the open-circuit voltage. Even low ion densities can have an impact on the electronic landscape when both cations and anions are considered as mobile. Moreover, we find that all measured ionic defects fulfil the Meyer–Neldel rule with a characteristic energy connected to the underlying ion hopping process. These findings support a general categorization of defects in halide perovskite compounds.
Bibliographical noteFunding Information:
C.D. and S.R. acknowledge financial support by the Bundesministerium für Bildung und Forschung (BMBF Hyper project, contract no. 03SF0514C) and thank their project partners from the University of Würzburg and ZAE Bayern for interesting discussions. Y.W.W. thanks Sunghyun Kim for assistance. Via our membership of the UK’s HEC Materials Chemistry Consortium, which is funded by EPSRC (EP/L000202), this work used the ARCHER UK National Supercomputing Service (http://www.archer.ac.uk). This work was also supported by a National Research Foundation of Korea (NRF) grant funded by the Korean government (MSIT) (no. 2018R1C1B6008728). Y.V. and C.D. thank the DFG for generous support within the framework of SPP 2196 project (PERFECT PVs). This project has received funding from the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (ERC Grant Agreement no. 714067, ENERGYMAPS).
All Science Journal Classification (ASJC) codes
- Biochemistry, Genetics and Molecular Biology(all)
- Physics and Astronomy(all)