DOI: https://doi.org/10.29363/nanoge.emlem.2023.008
Publication date: 18th August 2023
Halide perovskites are of immense importance due to their excellent light-absorbing and emitting properties, holding great promise in the field of advanced and clean energy technologies. One of the main mechanisms governing their unique properties at finite temperatures is the effect of electron-phonon coupling. However, achieving accurate simulations of electron-phonon coupling in these compounds requires understanding the effects of anharmonicity and polymorphism, as well as the intricate nature of their potential energy surface. In this talk, I will show how the anharmonic special displacement method (A-SDM) [1] allows for exploring anharmonic electron-phonon coupling in both layered and bulk halide perovskites. I will first demonstrate the importance of polymorphism in these compounds leading to strongly-coupled vibrational dynamics and strong modifications in the electron-phonon matrix elements [2]. Then, I will discuss that polymorphism holds the answer to elucidating the smooth evolution of the band gap with temperature around phase transitions [2]; a behavior that has proven challenging to understand thus far. Our work establishes a comprehensive framework that enables precise simulations of halide perovskites' carrier mobilities, excitonic spectra, and polaron physics.
M.Z. acknowledges funding from the European Union’s Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie Grant Agreement No. 899546. This research was also funded by the European Union (project ULTRA-2DPK / HORIZON-MSCA-2022-PF-01 / Grant Agreement No. 101106654). Views and opinions expressed are however those of the authors only and do not necessarily reflect those of the European Union or the European Commission. Neither the European Union nor the granting authority can be held responsible for them. J.E. acknowledges financial support from the Institut Universitaire de France. The work at institute FOTON and ISCR was supported by the European Union’s Horizon 2020 research and innovation program under grant agreement 861985 (PeroCUBE) and grant agreement 899141 (PoLLoC).
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