Capturing Charge Carrier Recombination Heterogeneity in Time-Resolved Photoluminescence Decays of Perovskite Thin Films
Margherita Taddei a, Sarthak Jariwala a, Shaun Gallagher a, Robert J. Westbrook a, David S. Ginger a
a Department of Chemistry, University of Washington, Seattle, WA, 98195-1700, USA
International Conference on Hybrid and Organic Photovoltaics
Proceedings of International Conference on Hybrid and Organic Photovoltaics (HOPV23)
London, United Kingdom, 2023 June 12th - 14th
Organizers: Tracey Clarke, James Durrant and Trystan Watson
Poster, Margherita Taddei, 148
Publication date: 30th March 2023

Time-resolved photoluminescence (TRPL) is a powerful technique for probing the properties of halide perovskite semiconductors, which have shown great potential for use in optoelectronic devices.[1],[2] However, interpreting TRPL decays can be challenging, as the decay curves can be influenced by a variety of physical factors.[3],[4] In this paper, we discuss commonly observed experimental PL decays, their likely physical origin, and common errors made when analyzing such data.

First, we point out that at low injection (low light intensity), high-quality (low defects) halide perovskites often show pseudo-first-order kinetics, consistent with classic minority carrier lifetimes. This observation can be used to extract information about the recombination processes that are occurring in the material.

Second, we discuss non-single-exponential decays that are often observed at low excitation intensity. These decays are typically a result of spatial heterogeneity in these polycrystalline samples. The resulting decay curves can often be well fit by stretched exponentials, which provide information about the distribution of carrier lifetimes in the material.

Third, we highlight that the PL decay kinetics can be sensitive to the excitation wavelength due to non-uniform carrier generation and diffusion, as well as surface recombination. This effect can be used to extract information about the carrier dynamics in the material.

Finally, we emphasize that failure to account for one or more of these factors can lead to erroneous results. By combining both experimental data and simulation, we demonstrate how to account for the above factors and extract reasonable values for parameters such as non-radiative losses. Our results provide important insights into how to best interpret TRPL data in halide perovskite semiconductors and will be useful for researchers working in this field.

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