Publication date: 15th December 2025
Understanding interfacial charge transfer dynamics in photoelectrochemical (PEC) systems is essential for optimizing the performance of semiconductor-based photoelectrodes. In this work, we systematically investigate electron transfer from the conduction band minimum (CBM) of a p-type semiconductor to redox states in the electrolyte under AM1.5G, as described by the Gerischer charge transfer model [1]. This framework considers the energetic overlap between the semiconductor CBM and a Gaussian distribution of redox states, defined by the reorganization energy (λ).
Here in this study, we focus on p-type Ag-alloyed Cu(In,Ga)Se2 (ACIGS) photocathodes and demonstrate that their PEC response is strongly governed by the alignment between the CBM and the redox energy distribution of protons (H+) in the electrolyte. A compositional series with varying Ag-to-(Ag+Cu) atomic ratios (AAC) is examined, revealing that shifts in CBM position relative to λ significantly affect interfacial charge transfer efficiency.
By fitting chopped-light linear sweep voltammetry (LSV) responses of ACIGS photocathodes with various AAC using the Gerischer model, we quantitatively extract key physical parameters including λ, CBM position, charge transfer rate constant (k0), and the effective photovoltage (EPh). The best-performing composition (AAC = 20%) shows the strongest overlap between CBM and λ, with a minimal energy offset (~30 meV), supporting highly efficient charge transfer and validating the model.
Overall, this study provides a quantitative application of the Gerischer charge transfer framework, offering valuable insight into the relationship between interfacial energetics and PEC performance, and guiding the rational design of high-efficiency photocathodes.
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