Photosystem I (PS I) is a transmembrane protein that assembles perpendicular to the membrane, and performs light harvesting, energy transfer, and electron transfer to a final, water‐soluble electron acceptor. We present here a supramolecular model of it formed by a bicationic oligofluorene 12+ bound to the bisanionic photoredox catalyst eosin Y (EY2−) in phospholipid bilayers. According to confocal microscopy, molecular modeling, and time dependent density functional theory calculations, 12+ prefers to align perpendicularly to the lipid bilayer. In presence of EY2−, a strong complex is formed (Ka=2.1±0.1×106 m−1), which upon excitation of 12+ leads to efficient energy transfer to EY2−. Follow‐up electron transfer from the excited state of EY2− to the water‐soluble electron donor EDTA was shown via UV–Vis absorption spectroscopy. Overall, controlled self‐assembly and photochemistry within the membrane provides an unprecedented yet simple synthetic functional mimic of PS I.

Invited for the cover of this issue are Andrea Pannwitz, Sylvestre Bonnet and co‐workers at Leiden University and Johns Hopkins University. The image depicts an observer watching over a lipid bilayer “landscape” and a sky full of luminescent giant vesicles. Read the full text of the article at 10.1002/chem.202003391.

A transmembrane dye and an energy accepting dye were implemented in lipid bilayers of liposomes and giant vesicles. Light‐induced energy transfer and transmembrane arrangement can be observed with luminescence spectroscopy, dynamic light scattering and confocal microscopy, supported by time‐dependent DFT calculations and molecular dynamics simulation. More information can be found in the Full Paper by A. Pannwitz, S. Bonnet, et al. on page 3013.