Publication date: 22nd July 2026
Unlike conventional semiconductor materials, metal halide perovskites (MHP) possess soft and ionic crystal structures leading to several unique features like facile ion migration, self-healing, elasticity, and memory. Within this dynamic system, external stimuli like high photon doses, electron beams, electrical bias, and mechanical stress induce structural changes and alter associated optoelectronic properties. Therefore, it is crucial to investigate the structure-photophysics relationship in these materials, especially in operational devices like solar cells, where surface-sensitive methods such as scanning electron microscopy fall short due to the layered structure. Moreover, electron and X-ray-based analytical techniques are often invasive, altering the device properties.
To address these challenges, we developed Correlation Clustering Imaging (CLIM)1,2, a novel noninvasive method that utilizes photoluminescence fluctuations to reveal contrasts associated with defect dynamics in semiconductor materials. CLIM images of perovskite thin films show one-to-one matching with the grains in SEM images captured at the same locations. Particularly noteworthy is the application of CLIM to high-efficiency photovoltaic devices, uncovering previously unnoticed photoluminescence intensity fluctuations that strongly depend on the device's operational regime. CLIM coupled with quasi-Fermi level splitting (QFLS) mapping provides rationale for the evolving landscape of device performance through mechanistic understanding of charge carrier dynamics.
These findings deepen our understanding of device efficiency, structure, and degradation — knowledge critical for the rational design of next-generation devices. Requiring only a standard wide-field microscope and an open-source, user-friendly algorithm, CLIM is broadly applicable and poised to become an important tool for materials chemists, engineers, and device scientists alike.
S.S. acknowledges the support of Marie Skłodowska-Curie postdoctoral fellowship (No. 101151427, SPS_Nano) from the European Union’s Horizon Europe program, short stay abroad grant (K257023N) and travel grant (K147824N) from Research Foundation-Flanders (FWO)
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