The photosynthetic protein, photosystem I (PSI), has been used as a photoactive species within a host of biohybrid photoelectrochemical systems. PSI multilayer films at electrode surfaces provide greatly improved solar energy conversion relative to homologous monolayer films. While the photocatalytic effect of PSI multilayers has been theorized as an electrolyte-mediated mechanism, no comprehensive, first-principles modeling study has been presented. In this work, we develop and optimize an electrochemical reaction-diffusion model to replicate the significant electrochemical, physicochemical, and transport processes that underpin photocurrent development of a PSI multilayer film. We use this model to provide strong evidence that PSI's terminal cofactors rapidly exchange electrons with diffusible mediators and stimulate photocurrent principally due to alteration of mediator concentrations at a solution-electrode interface as governed by Butler-Volmer kinetics. Our fitted model accurately replicates photocurrent trends under a variety of conditions, including variable applied bias and PSI multilayer film thickness.
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