Publication date: 15th December 2025
Electrochemistry and spectroelectrochemistry are powerful tools to probe the optoelectronic properties of lead-halide perovskites and understand the working princinples of related hybrid architectures.[1] Spectroelectrochemical measurements enable the determination of reliable band diagrams, identification of trap-state energies and densities and to understand the corrosion pathways and degradation mechanism in these systems. From these insights we propose a set of boundary conditions and recommended protocols to perform electrochemical studies on lead-halide perovskites. Coupling ultrafast transient absorption specroscopy with electrochemical methods allow probing charge transfer processess on the femtosecond to nanosecond timescales.[2] However the intrinsic instability of lead-halide perovskites restricts the choice of compatible solvents and electrolytes to conduct these measurements. When these studies are extended to highly confined 2D systems the presence of a bulky organic cations in the structure (e.g., buthylammonium, phenethylammonium) further complicates the already complex picture.
The overarching goal of my presentation if to define a stability window for electrochemical testing of various lead-halide perovskite systems. In the first part general principles of performing spetroelectrochemical measurements on 3D, 2D lead-halide perovskite based systems will be outlined. The influence of material composition (e.g., nature of organic cations, halide anions) on the electrochemical stability will be discussed. The insights gained through spectroelectrochemistry combined with ultraviolet photoelectron spectroscopy and surface photovoltage spectroscopy, was used to determine precise band positions and reveal the presence of mid-gap states within these materials.
In the second part of the use of in situ transient spectroelectrochemistry will be demonstrated, where the role of thermodynamic band offsets in hole transfer will be evaluated using FA0.83Cs0.17Pb(IxBr1-x)3 films on mesoporous NiO. Systematic tuning of the valence band revealed that larger valence band offsets enhance hole extraction. In situ transient spectroelectrochemistry further showed that applying negative bias accelerates hole transfer, with stronger effects observed for compositions exhibiting larger offsets. These findings clarify how band alignment governs hole extraction at NiO/perovskite interfaces and provide design principles for more efficient optoelectronic devices.[3]
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