Single Best Fits Can Be Misleading: Resolving Common Trapping Signatures across FA--Cs Perovskites

Abstract

Identifying defects responsible for non-radiative recombination in metal-halide perovskites remains challenging, with no common defect signatures established across compositions. Here, we combine fluence-dependent time-resolved photoluminescence, full Shockley--Read--Hall modelling and Bayesian posterior inference across an FA${}_{1-x}$Cs${}_x$PbI${}_3$ compositional series. We show that trap occupation governs carrier dynamics and defect-parameter identifiability in semiconducting materials: weakly occupied states exhibit electron-capture-coefficient--trap-density degeneracies, whereas trap filling lifts them. In our perovskite systems, a non-degenerate signature $T\beta$, characterized by a strongly asymmetric ${\beta }_p/{\beta }_n$ capture-coefficient ratio, occurs across all compositions, suggesting substantial trap filling is a general feature of perovskite carrier dynamics. We further identify $T\alpha$ as a shared, device-performance-limiting non-radiative recombination channel, while a shallow $T\epsilon$ signature unique to FAPbI${}_3$ produces the largest steady-state non-radiative recombination rate and is consistent with the previously observed high stacking-fault density of this composition. This framework therefore provides a basis for comparing trapping signatures across different semiconducting materials at room temperature.

Supporting code is in: https://github.com/MimaxSimm/FACs-TrapSignatures DOI code: https://doi.org/10.5281/zenodo.22791960 DOI data: https://doi.org/10.5281/zenodo.22791430