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Mimicking Photosystem I with a Transmembrane Light Harvester and Energy Transfer‐Induced Photoreduction in Phospholipid Bilayers

Andrea Pannwitz, Holden Saaring, Nataliia Beztsinna, Xinmeng Li, Maxime A. Siegler, Sylvestre Bonnet

2020Chemistry - A European Journal26 citationsDOIOpen Access PDF

Abstract

Abstract 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 1 2+ bound to the bisanionic photoredox catalyst eosin Y (EY 2− ) in phospholipid bilayers. According to confocal microscopy, molecular modeling, and time dependent density functional theory calculations, 1 2+ prefers to align perpendicularly to the lipid bilayer. In presence of EY 2− , a strong complex is formed (K a =2.1±0.1×10 6 m −1 ), which upon excitation of 1 2+ leads to efficient energy transfer to EY 2− . Follow‐up electron transfer from the excited state of EY 2− 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.

Topics & Concepts

PhotochemistryElectron transferChemistryLipid bilayerBilayerPhotosystem IEosin YElectron acceptorExcited statePhospholipidSpectroscopyMembranePhotosystem IIPhotosynthesisCatalysisPhotocatalysisOrganic chemistryNuclear physicsQuantum mechanicsBiochemistryPhysicsPhotosynthetic Processes and MechanismsPhotoreceptor and optogenetics researchSpectroscopy and Quantum Chemical Studies
Mimicking Photosystem I with a Transmembrane Light Harvester and Energy Transfer‐Induced Photoreduction in Phospholipid Bilayers | Litcius