Publication date: 22nd July 2026
Photoelectrochemical (PEC) water oxidation using semiconductor photoanodes represents a promising pathway for sustainable hydrogen production. However, accurately quantifying bulk transport, interfacial recombination, and charge-transfer kinetics remains a challenge due to the limitations of existing optoelectronic models. Many traditional frameworks, such as the widely used two-capacitor model, assume perfect electron extraction or fail to maintain self-consistency between steady-state and dynamic small-perturbation measurements. Furthermore, they often neglect the critical distinction between the internal quasi-Fermi-level splitting and the external applied voltage under illumination.
To resolve these issues, we present a comprehensive, self-consistent analytical model designed to interpret both steady-state current–voltage characteristics and small-perturbation responses across the time and frequency domains. The framework explicitly accounts for imperfect electron extraction at the collecting contact and links bulk recombination directly to the internal voltage profile. The physical validity of the analytical model is corroborated by full drift-diffusion simulations, demonstrating excellent agreement across varying light intensities and bias potentials.
Applying this model to experimental data for a hematite photoanode yields specific charge-transfer and extraction parameters near the 1 sun open-circuit potential. The framework, which links extraction velocity to electronic mobility, accounts for the characteristic linear dependence of photocurrent on voltage observed in hematite, offering a robust tool for analyzing diverse photoelectrochemical systems.
We acknowledge that this work is funded by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) – project number 539945054. We also acknowledge support from the Helmholtz Association via the programme-oriented funding (POF IV) and the SolarTap project. Open access publication funded by the DFG – 491111487.
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