US-France Cooperative Research: Electronic Spectroscopy and Photochemistry of Transition Metal Complexes Studied via Coupled-Cluster Calculations and Wavepacket Propagation

在这个为期三年的美法合作研究项目中，将利用量子化学计算和波包动力学来研究飞秒激光实验中观察到的一系列小过渡金属羰基和过渡金属-羰基离子的光解动力学。主要目的是分析在过渡金属分子中观察到的并发破碎方案的机制。该项目由佛罗里达大学的罗德尼·巴特利特（Rodney Bartlett）领导的美国研究人员和法国斯特拉斯堡路易斯·巴斯德研究所的尚塔尔·丹尼尔（Chantal Daniel）和阿兰·斯特里奇（Alain Strich）领导的法国研究人员共同参与，利用了他们的专业知识和互补的理论方法。斯特拉斯堡小组将应用于过渡金属配合物的光谱和光反应性，高度相关的变分/微扰方法和波包传播。佛罗里达大学将实施耦合簇方法应用于光谱学和小分子的分子性质。最近，这个小组将他们的方法应用于扩展有机系统中的亚基。研究人员将解决有关导致选择性断键的化学活性电子态之间的差异以及确定并发断裂过程的时间尺度和分支比例的基本问题。国际上的努力将促进我们对过渡金属化合物光化学的理解。这项工作与物理、无机和有机金属化学和催化有关。此外，美国化学研究生将受益于前沿化学研究领域优秀的国际团队的培训。该项目由美国国家科学基金会（NSF）和法国国家科学研究中心（CNRS）联合支持。美国国家科学基金会将为美国研究人员和研究生访问法国提供支持。国家科学研究中心为法国队访问美国提供了类似的资助。

0340787BartlettIn this three-year U.S.-France cooperative research project, photodissociation dynamics of a series of small transition metal carbonyls and transition metal-carbene ions observed in femtosecond laser experiments will be investigated using quantum chemical calculations supplemented by wave packet dynamics. The main objective is to analyze the mechanism underlying concurrent fragmentation schemes observed in transition metal molecules. This project involves U.S. researchers led by Rodney Bartlett at the University of Florida and French researchers led by Chantal Daniel and Alain Strich at the Institut Louis Pasteur in Strasbourg, France and takes advantage of their combined expertise and complementary theoretical methods. The Strasbourg group will apply to spectroscopy and photoreactivity of transition metal complexes highly correlated variational/perturbational methods and wave packet propagations. The University of Florida will implement coupled cluster methods applied to spectroscopy and molecular properties of small molecules. Most recently this group has applied their methods to subunits in extended organic systems. The investigators will solve fundamental questions concerning the differentiation between chemically active electronic states that lead to selective bond breaking and the determination of time scales and branching ratios of concurrent fragmentation processes. The international effort will advance our understanding of photochemistry of transition metal compounds. This work is relevant for physical, inorganic and organometallic chemistry and catalysis. In addition, U.S. graduate students in chemistry will benefit from training with an excellent international team in chemistry research at the frontier.The project is jointly supported by the National Science Foundation (NSF) and the Centre National de la Recherche Scientifique (CNRS). NSF will provide support for visits by the U.S. investigators and graduate students to France. The CNRS provides similar funding for visits to the United States by the French team.