Proceedings of MATSUS Spring 2024 Conference (MATSUS24)
DOI: https://doi.org/10.29363/nanoge.matsus.2024.157
Publication date: 18th December 2023
Following the emergence of lead halide perovskites (LHPs) as materials for efficient solar cells, research has progressed to explore stable, abundant and non-toxic alternatives. However, the performance of such lead-free perovskite-inspired materials (PIMs) still lags significantly behind that of their LHP counterparts. For bismuth (Bi)-based PIMs, one significant reason is a frequently observed ultrafast charge-carrier localization (or self-trapping). It has been suggested that self-trapping in Cs2AgBiBr6 originates from strong lattice deformation potential imparted by bismuth along with the presence of soft silver-halide bonds. Given that self-trapping places a fundamental limit on the performance of materials, investigating the influence of chemical composition on the charge-carrier dynamics is highly topical.
This work aims to understand whether the presence of Bi or Ag-halide bonds is in fact crucial to the emergence of self-trapped states. This was done through a dual study of charge-carrier dynamics in BiOI and (AgI)x(BiI3)y thin films. Our investigation reveals that despite possessing a low and strong electron-phonon coupling, there is no ultrafast localisation in BiOI. Instead, by unravelling the early and long-time charge-carrier dynamics in BiOI, we find that the material performance is limited by the presence of multi-phonon emission mediated non-radiative channels in the material.
On the other hand, ultrafast localisation is persistent across both mixed Ag-Bi iodides and BiI3. Thus, the presence of Bi and/or Ag-halide bonds alone cannot account for self-trapping in these materials. We find that a delicate interplay between chemical composition and crystal and band structures determine the charge-carrier dynamics in (AgI)x(BiI3)y. Overall, our dual study addresses crucial gaps in understanding the limitations of Bi-based PIMs and educate future material design.
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