Proceedings of MATSUS Spring 2024 Conference (MATSUS24)
DOI: https://doi.org/10.29363/nanoge.matsus.2024.272
Publication date: 18th December 2023
Lead-free double perovskites are emerging as an alternative to toxic lead-based perovskites for both light-emitting and light harvesting applications. Owing to the soft and polar nature, lattice deformations in metal halide perovksites can strongly couple to charge carriers upon photoexcitation. In contrast to lead-based perovskites, double perovskites exhibit intrinsic defects (Ag-vacancies), resulting in bound excitons with giant oscillator strengths. We utilize femtosecond pump-probe spectroscopy to investigate the dynamics of bulk and localized coherent phonons in spherical Cs2AgBiBr6 double perovskite nanocrystals at cryogenic temperatures. In this study, we observe that optically launched bulk lattice vibrations modify the spectral position of the bound excitonic resonance. Surprisingly, we found that this Ag-vacancy bound exciton is modulated in its giant oscillator strength. We argue that this is a consequence of an optically generated vibrational wave-packet localized at this very Ag-vacancy. This optically induced and spatially localized lattice shaking could become potentially useful for initiating photochemical or photocatalytic reactions with atomic precision.
We acknowledge financial support by the Bavarian State Ministry of Science and Arts and by the LMU Munich through the grant “Solar Technologies go Hybrid (SolTech). We thank local research clusters and centers such as CeNS for providing communicative networking structures. F. H. acknowledges the China Scholarship Council. T.D. acknowledges the Department of Science & Technology (DST) and the Science and Engineering Research Board (SERB) for the Ramanujan Fellowship Award (RJF/2021/000125). We acknowledge and thank Matthias Kestler for helpful discussions.
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