Are Shockley-Read-Hall and ABC models valid for lead halide perovskites?

Abstract

Metal halide perovskites are an important class of emerging semiconductors. Their charge dynamics is poorly understood due to limited knowledge of defect physics and charge recombination mechanisms. Nevertheless, classical ABC and Shockley-Read-Hall (SRH) models are ubiquitously applied to perovskites without considering their validity. Herein, an advanced technique mapping photoluminescence quantum yield (PLQY) as a function of both the excitation pulse energy and repetition frequency is developed and employed to examine the validity of these models. While ABC and SRH fail to explain the charge dynamics in a broad range of conditions, the addition of Auger recombination and trapping to the SRH model enables a quantitative fitting of PLQY maps and low-power PL decay kinetics, and extracting trap concentrations and efficacies. Higher-power PL kinetics requires the inclusion of additional non-linear processes. The PLQY mapping developed herein is suitable for a comprehensive testing of theories and is applicable to any semiconductor.

Supplementary Information available at https://cloudstore.zih.tu-dresden.de/index.php/s/t5gBPJgwZiwfRRA

References in corpus (3)

• Shining Light on Photoluminescence Properties of Metal Halide Perovskites
• Probing the ionic defect landscape in halide perovskite solar cells
• Insights from Device Modeling of Perovskite Solar Cells

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• Resolving nonlinear recombination dynamics in semiconductors via ultrafast excitation correlation spectroscopy: Photoluminescence versus photocurrent detection
• The model of photoswitching in lead-halide perovskite microcrystals
• A Review on Improving PSC Performance through Charge Carrier Management: Where We Stand and What's Next?