Slow diffusion and long lifetime in metal halide perovskites for photovoltaics

TL;DR

This study investigates the surprisingly slow charge carrier diffusion and long lifetimes in metal halide perovskites, revealing that high efficiency persists despite slow diffusion, due to complex recombination dynamics.

Contribution

The paper introduces an improved model for analyzing time-resolved photoluminescence that accounts for transport, photon recycling, and traps, applied to various perovskite materials.

Findings

Charge carrier diffusion coefficient around 5x10^-3 cm^2/s.

Band-to-band recombination rate close to radiative limit.

High power conversion efficiency despite slow diffusion.

Abstract

Metal halide perovskites feature excellent absorption, emission and charge carrier transport properties. These materials are therefore very well suited for photovoltaics applications where there is a growing interest. Still, questions arise when looking at the unusual long carrier lifetime that, regarding the micrometric diffusion length, would imply a very low diffusion coefficient as compared to commonly used photovoltaic absorbers. In this paper, we provide an experimental insight into this long lifetime of charge carriers in slow-motion. Our approach relies on an improved model to analyze time-resolved photoluminescence decays at multiple fluence levels that includes charge carrier transport, photon recycling, and traps dynamics. The model is verified on different interface properties. Moreover, we investigate various perovskite absorbers such as mixed alloys with cesium content. For most of the perovskite based materials we analyzed, the band-to-band recombination rate remains close to the radiative limit, leading to the expected sub-microsecond lifetime. The slow diffusion of charge carriers is observed with values of the diffusion coefficient D around 5x10-3 cm2/s. Nonetheless, the power conversion efficiency remains high. The observations might be related to the debated coexistence of a direct and indirect bandgap slowing down the recombination process.