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Photosystem 1 (PS1) triggers the most energetic light‐induced charge‐separation step in nature and the in vivo electron‐transfer rates approach 50 e− s−1 PS1−1. Photoelectrochemical devices based on this building block have to date underperformed with respect to their semiconductor counterparts or to natural photosynthesis in terms of electron‐transfer rates. We present a rational design of a redox...
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