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Quantifying Evolving Defect Parameters in Metal Halide Perovskites via the Measurement and Modeling of Power-Dependent Transient Photoluminescence
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DOI：10.1002/aenm.202504811.png)
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Abstract
En 中文
Dynamic photoinduced defect states in metal halide perovskites (MHPs) critically govern the non-equilibrium photophysics, metastability, and long-term performance of optoelectronic devices, such as solar cells. This metastability is evident in steady-state photoluminescence experiments, where the amplitudes increase or decrease depending on the environmental and excitation conditions. Here, we combine excitation-dependent time-resolved photoluminescence (trPL) measurements with parameter estimation via Bayesian optimization coupled with a full Shockley–Read–Hall and diffusion model to quantitatively track defect state formation in Cs0.05FA0.95PbI3 thin films, under continuous 1 sun illumination. This methodology is applied to quantify the evolution of defect distributions in absorbers with two distinct initial optoelectronic qualities, leveraging the sensitivity of trPL decays to defect-assisted non-radiative recombination processes. We show that 21 h of continuous illumination causes the slopes of the differential-lifetime/mean carrier-density plots to converge from initially distinct decay behaviors, which we interpret as a convergence of dominant recombination mechanisms following irradiation. The fitting results further suggest the emergence of trapping species with highly asymmetric capture cross-section ratios. Overall, this study establishes a general diagnostic methodology for tracking carrier-induced degradation pathways in perovskites and other emerging semiconductors.
Keywords:
carrier dynamics
defect parameters
perovskite defects
time resolved photoluminescence
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