Local Disorder and Electron-Anharmonic Phonon Coupling in Metal Halide Perovskites

Marios Zacharias^a, Jacky Even^a, George Volonakis^b, Feliciano Giustino^c^,^d

^aUniv Rennes, INSA Rennes, CNRS, Institut FOTON - UMR 6082, F-35000 Rennes, France.

^bUniv Rennes, ENSCR, INSA Rennes, CNRS, ISCR - UMR 6226, F-35000 Rennes, France.

^cOden Institute for Computational Engineering and Sciences, The University of Texas at Austin, Austin, Texas 78712, USA.

^dDepartment of Physics, The University of Texas at Austin, Austin, Texas 78712, USA.

Materials for Sustainable Development Conference (MATSUS)
Proceedings of MATSUS Spring 2024 Conference (MATSUS24)

#PerFut24 - The Future of Metal Halide Perovskites: Fundamental Approaches and Technological Challenges

Barcelona, Spain, 2024 March 4th - 8th

Organizers: Annalisa Bruno, Iván Mora-Seró and Pablo P. Boix

Oral, Marios Zacharias, presentation 055
DOI: https://doi.org/10.29363/nanoge.matsus.2024.055
Publication date: 18th December 2023

Metal halide perovskites are of immense importance due to their excellent optoelectronic properties, holding great promise in the field of advanced and clean energy technologies. One of the fundamental mechanisms governing their physical properties is the interplay of electron-phonon coupling with the strong lattice anharmonicity and their inherent locally disordered structure [1,2]. To understand the consequences of these effects, we have recently introduced a powerful theoretical framework that allows to capture anharmonic electron-phonon coupling in these intrinsically polymorphous compounds [3,4]. In this talk, I will demonstrate our methodology for both inorganic and hybrid halide perovskites and show that (i) local disorder is at the origin of overdamped and strongly coupled anharmonic phonons, (ii) low-energy optical vibrations dominate electron–phonon renormalized band gaps, departing from a simplified picture of a Fröhlich interaction, and (iii) local disorder is the key to explain the monotonic increase of the band gap across phase transitions. Our work provides a new perspective for the interpretation of perovskite materials fundamentals as well as opens the way for efficient simulations of halide perovskites' key properties, like carrier mobilities, excitonic spectra, and polaron physics.

References:

[1] [1] Tamarat, P., Prin, E., Berezovska, Y. Zacharias M. et al. Universal scaling laws for charge-carrier interactions with quantum confinement in lead-halide perovskites. Nat Commun 14, 229 (2023).

[2] [2] Dirin D. N., Vivani A., Zacharias M. et al, Intrinsic Formamidinium Tin Iodide Nanocrystals by Suppressing the Sn(IV) Impurities, Nano Lett. 23, 5, 1914 (2023).

[3] [3] Zacharias, M., Volonakis, G., Giustino, F Even J. Anharmonic electron-phonon coupling in ultrasoft and locally disordered perovskites. npj Comput. Mater. 9, 153 (2023)

[4] [4] Zacharias, M., Volonakis, G., Giustino, F Even J. Anharmonic lattice dynamics via the special displacement method, Phys. Rev. B 108, 035155 (2023).

Acknowledgements:

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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