A biomimetic assembly of folded photosystem I monolayers for an improved light utilization in biophotovoltaic devices.

[Display omitted] • A bioelectrode constituted by a folded assembly of PSI monolayers is introduced. • The influence of incident light angle on photocurrent generation is investigated. • The folded assembly is shown to provide an improved utilization of incident light. In the fabrication of photosystem I (PSI)-based biodevices, the use of multilayered architectures aims to maximize the absorption of incident light that can be converted into high-energy electrons. The challenge in this strategy is to overcome the large driving force imposed by the photoinduced potential difference between the two terminal redox centers that are located at opposite sides of PSI, which translates into charge recombination resulting in sub-optimal performance of commonly implemented systems. The integration of PSI monolayers with electrodes using the Langmuir-Blodgett technique enables a preferential anisotropic orientation of PSI in a tightly packed structure, which minimizes short-circuiting processes and aids to improve the performance of PSI-based biodevices. However, the practical application of PSI monolayer-based biodevices is limited due to the small loading of immobilized PSI molecules, leading to overall low utilization of incident light. Inspired by the stacked arrangements of thylakoids in nature, we demonstrate the fabrication of biomimetic structures using multiple PSI monolayers assembled into a folded architecture to improve light absorption and with that the performance of the overall photoelectrode. [ABSTRACT FROM AUTHOR]