Investigating the ultrafast dynamics of natural and artificial light harvesting

植物，藻类和某些细菌有效地捕获地球上丰富的阳光，以推动光合作用-将二氧化碳和水转化为植物生长所需的单糖的过程。虽然对自然光合作用的宏观理解已经建立，但支撑光合作用所谓的“设计原理”的微观细节尚未完全详细。包封捕光叶绿素部分的蛋白质的几个作用是公认的，但叶绿素和蛋白质残基之间的特定分子相互作用，引起其独特的浴响应已经回避了实验研究。将研究具有已知X射线晶体结构的模型蛋白质，其仅包含一个或两个可见发色团，以揭示蛋白质的“浴”动力学作为结合残基和蛋白质口袋的函数。分子结构和总功率转换效率之间的关系仅开始出现于过多的材料有机体异质结或半导体材料。在所有情况下，吸收的光都被用来诱导电荷分离成电子和空穴，但这种过程的机制和位置仍然模糊不清。超快多维光谱学（如二维电子光谱学）将被用来探索这些现象，创建一个具有飞秒时间分辨率（1 fs = 1百万分之十亿分之一秒）的组成分子之间的能量流图。

Plants, algae and certain bacteria efficiency capture the abundant sunlight incident on the Earth to drive photosynthesis- the process of converting carbon dioxide and water into simple sugars used for plant growth. Whilst a macroscopic understanding of natural photosynthesis has been established, microscopic details that underpin the so-called "design principles" of photosynthesis have yet to be fully detailed. Several roles for the protein that encapsulates the light harvesting chlorophyll moieties are recognised, but the specific molecular interactions between chlorophyll and protein residues that give rise to their unique bath response have eluded experimental studies. Model proteins with known x-ray crystal structures, that contain only one or two visible chromophores will be investigated to reveal the "bath" dynamics of the protein as a function of the binding residue and protein pocket.Man-made efforts to efficiency harness the solar flux have been far less effective, with relationships between the molecular structure and overall power conversion efficiencies only starting to emerge for a plethora of materials such as organic bulk-heterojunctions or semi-conducting materials. In all instances, the absorbed light is used to induce charge separation into electrons and holes, but the mechanism and location for such processes remain nebulous.Ultrafast multidimensional optical spectroscopies such as 2D electronic spectroscopy will be used to explore these phenomena, creating a map of energy flow between constituent molecules with femtosecond time resolution (1 fs = 1 millionth billionth of a second).