Stones Richard, Hossein-Nejad Hoda, van Grondelle Rienk, Olaya-Castro Alexandra
Department of Physics and Astronomy , University College London , Gower Street , London , WC1E 6BT , UK . Email:
Department of Physics and Astronomy , VU University , 1081 HV Amsterdam , The Netherlands.
Chem Sci. 2017 Oct 1;8(10):6871-6880. doi: 10.1039/c7sc02983g. Epub 2017 Aug 4.
The photosystem II reaction centre is the photosynthetic complex responsible for oxygen production on Earth. Its water splitting function is particularly favoured by the formation of a stable charge separated state a pathway that starts at an accessory chlorophyll. Here we envision a photovoltaic device that places one of these complexes between electrodes and investigate how the mean current and its fluctuations depend on the microscopic interactions underlying charge separation in the pathway considered. Our results indicate that coupling to well resolved vibrational modes does not necessarily offer an advantage in terms of power output but can lead to photo-currents with suppressed noise levels characterizing a multi-step ordered transport process. Besides giving insight into the suitability of these complexes for molecular-scale photovoltaics, our work suggests a new possible biological function for the vibrational environment of photosynthetic reaction centres, namely, to reduce the intrinsic current noise for regulatory processes.
光系统II反应中心是地球上负责产生氧气的光合复合体。其水裂解功能特别有利于形成稳定的电荷分离态,这一过程始于一个辅助叶绿素。在此,我们设想了一种将这些复合体之一置于电极之间的光伏器件,并研究平均电流及其涨落如何依赖于所考虑路径中电荷分离的微观相互作用。我们的结果表明,与分辨率良好的振动模式耦合在功率输出方面不一定具有优势,但可导致具有抑制噪声水平的光电流,这表征了一个多步有序传输过程。除了深入了解这些复合体在分子尺度光伏方面的适用性外,我们的工作还表明光合反应中心的振动环境可能具有一种新的生物学功能,即降低调节过程中的固有电流噪声。