Strong self-trapping by deformation potential limits photovoltaic performance in bismuth double perovskite

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Abstract

Bismuth-based double perovskite Cs2AgBiBr6is regarded as a potential candidate for low-toxicity, high-stability perovskite solar cells. However, its performance is far from satisfactory. Albeit being an indirect bandgap semiconductor, we observe bright emission with large bimolecular recombination coefficient (reaching 4.5 ± 0.1 × 10-11cm3s-1) and low charge carrier mobility (around 0.05 cm2s-1V-1). Besides intermediate Fröhlich couplings present in both Pb-based perovskites and Cs2AgBiBr6, we uncover evidence of strong deformation potential by acoustic phonons in the latter through transient reflection, time-resolved terahertz measurements, and density functional theory calculations. The Fröhlich and deformation potentials synergistically lead to ultrafast self-trapping of free carriers forming polarons highly localized on a few units of the lattice within a few picoseconds, which also breaks down the electronic band picture, leading to efficient radiative recombination. The strong self-trapping in Cs2AgBiBr6could impose intrinsic limitations for its application in photovoltaics.

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Wu, B., Ning, W., Xu, Q., Manjappa, M., Feng, M., Ye, S., … Sum, T. C. (2021). Strong self-trapping by deformation potential limits photovoltaic performance in bismuth double perovskite. Science Advances, 7(8). https://doi.org/10.1126/sciadv.abd3160

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