Publication date: 21st July 2025
Metal halide perovskites are highly promising materials for next-generation photovoltaics due to their exceptional optoelectronic properties and cost-effective fabrication. [1] Various ion substitution strategies have been explored to enhance the photovoltaic performance of methylammonium lead iodide (MAPI) films, including A-site ion substitution, B-site ion substitution, and X-site ion substitution. [2] In contrast to the tolerance and stability tailoring or electronically tuned modifications brought about by A-site and X-site ion substitution, the main change of B-site ion substitution is its influence on the fundamental vibrational and structural properties of the inorganic [PbI6]⁴⁻ octahedral network. [3] Compared to the isovalent ion substitution, heterovalent ion substitution is found to influence the sign of majority charge carriers. [4] In particular, the incorporation of antimony has been shown to improve the performance of MAPI devices by enhancing their optoelectronic properties, [5] while the underlying mechanism of such modification remains underexplored. Our study investigates the effect of antimony ion substitution on MAPI films using a combination of optical pump-terahertz probe spectroscopy (OPTP) and transient absorption spectroscopy (TA). We find that OPTP photoconductivity transients exhibit a fluence-dependent crossover that is absent in pristine MAPI. Conversely, TA results do not show this same crossover behavior. This difference strongly indicates a mobility-driven phenomenon, which we attribute to enhanced charge carrier localization with antimony ion substitution. This is also verified by the increase of radiative recombination rate and the reduction of charge carrier mobility, as the concentration of antimony ions grows. Our findings pave the way for understanding the effect of antimony ion substitution on the interaction between charge carrier localization and recombination, which is crucial for optimizing optoelectronic properties of perovskite thin films.
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