Time-resolved photoluminescence (TRPL) spectroscopy is a powerful technique to investigate excited charge carrier recombinations in semiconductors and molecular systems. The analysis of the TRPL decays of many molecular systems (e.g. molecules and organic materials) is usually fairly straightfoward and can be fitted with an exponential function allowing extraction of the rate constants. Due to the non-excitonic nature of charge carriers in lead halide perovskite materials coupled with the presence of localised trap states in their band-gap, the TRPL of these materials is much more complicated to interpret. Here we discuss two models used in the literature to simulate charge carrier recombinations and TRPL in perovskites. These models consider the bimolecular nature of direct electron-hole recombination but differ in their treatment of trap-mediated recombination with one model describing trapping as a monomolecular process whereas the other as a bimolecular process between free carriers and the available trap states. In comparison, the classical analysis of perovskite TRPL decay curves (using a sum of exponentials) can lead to misinterpretation. Here we offer some recommendations for meaningful measurements of lead halide perovskite thin-films. The fluence dependence as well as charge carrier accumulation due to incomplete depopulation of all photoexcited carriers between consecutive excitation pulses are discussed for both models.
Bibliographical noteKAUST Repository Item: Exported on 2020-12-14
Acknowledgements: We are grateful for the financial support of the EPSRC (EP/R016666/1 and EP/S001336/1) and both the EPSRC and Innovate UK for the SPECIFIC Innovation and Knowledge Centre and the European Regional Development Fund through the Welsh Government for support to the Seˆr Solar program. MLD is grateful for funding through the EPSRC GCRF SUNRISE project (EP/P032591/1). We would like to acknowledge the assistance provided by the European Regional Development Fund through the Welsh Government (80708), the Ser Solar
project via Welsh Government and Edinburgh Instruments.