COST D35 Collaboration Optically and electronically controlled states of metal-based molecular systems. Experiment and theory

国际合作项目“金属基分子系统的光学和电子控制状态”。实验和理论于2006年1月在新的成本行动D35中建立，从分子到分子器件：电子，光子，磁性和自旋电子行为的控制。该项目结合了11个领先的欧洲实验室在化学合成、最先进的激光光谱学、电化学和理论方面的努力，以全面理解和控制多组分金属基分子组装中的电子转移、电荷分离和电子效应的传输。伦敦大学玛丽皇后学院的伦敦小组在该计划中发挥着核心和主导作用，PI是该计划的协调员和D35行动的主席。申请的资金将使伦敦小组能够积极参与这一欧洲合作。我们将重点关注新的光活性含金属化合物。研究将从研究它们的结构和激发态的动态演变，到了解它们的弛豫过程，最后是光致电子转移。后一过程导致电荷分离和各种分子功能，适用于分子器件。通过了解和控制激发态特性和弛豫动力学，我们期望找到加速和控制转移和激发态电荷分离的方法。我们还将讨论过渡金属光物理的独特和相关特征，如亚皮秒系统间交叉到三重态，弛豫过程中多余能量的超快释放，广泛的介质重组等，其在分子器件中的应用潜力需要评估。这些复杂的任务将结合实验和理论研究，采用最先进的结构敏感时间分辨红外（TRIR）和拉曼光谱，皮秒x射线吸收，超快紫外-可见和荧光上转换光谱，以及现代量子化学和分子动力学计算技术。合作将扩大我们的合成基地，增加我们光物理研究的化学系统的范围，使我们能够将我们的实验工作与高水平的量子化学计算相结合，并为我们提供最先进的实验技术（超快时间分辨UV-Vis， x射线和2D-IR光谱，荧光上转换），其中一些在英国是不可用的。因此，此次合作的资金将使我们的实验设施、人力和专业知识成倍增加，从而有利于在英国以及合作的欧洲实验室进行的研究。

An international collaborative project entitled Optically and electronically controlled states of metal-based molecular systems. Experiment and theory was established in January 06 within the new COST Action D35 From Molecules to Molecular Devices: Control of Electronic, Photonic, Magnetic and Spintronic Behaviour . This project combines the efforts of 11 leading European laboratories in chemical synthesis, state-of-the-art laser spectroscopy, electrochemistry, and theory to achieve a comprehensive understanding and control of electron transfer, charge separation, and transmission of electronic effects in multicomponent metal-based molecular assemblies . The London group at Queen Mary, University of London plays a central and leading role in this programme, the PI being its coordinator and the chair of the D35 Action. The funding being applied for will enable the London group to participate actively in this European collaboration.We will focus on new photoactive metal-containing compounds. The research will proceed from investigations of the structures and dynamic evolution of their excited states to understanding of their relaxation processes and, finally, of photoinduced electron transfer. It is the latter process which leads to charge separation and various molecular functions, applicable in molecular devices. By understanding and controlling excited-state characters and relaxation dynamics, we expect to find means to accelerate and control transfer and excited-state charge separation. We will also address unique and relevant features of transition-metal photophysics, such as sub-picosecond intersystem crossing to triplet states, ultrafast release of excess energy during relaxation, extensive medium reorganization, etc., whose potential for applications in molecular devices needs to be assessed. These complex tasks will be approached by combined experimental and theoretical investigations, employing state-of-the-art structure-sensitive time-resolved IR (TRIR) and Raman spectroscopy, picosecond X-ray absorption, ultrafast UV-Vis and fluorescence up-conversion spectroscopy, together with modern quantum chemical and molecular dynamics computational techniques. Collaborations will expand our synthetic base, increase the range of chemical systems for our photophysical studies, allow us to combine our experimental work with high-level quantum chemical calculations, and provide us with an access to state-of-the art experimental techniques (ultrafast time-resolved UV-Vis, X-ray, and 2D-IR spectroscopy, fluorescence up-conversion), some of which are unavailable in the UK. Funding of this collaboration will thus multiply our experimental facilities, manpower and expertise to the benefit of the research performed in the UK, as well as in the collaborating European labs.