Modeling and Laser Control of Molecular Vibrational Energy Flow

伊利诺伊大学厄巴纳分校的Martin Grubele得到了实验物理化学计划的资助，继续他在有机分子中振动能量流方面的工作。 这涉及（1）将他的理论模型扩展到包括甲醇、吡咯、乙腈、乙烯酮和硫光气，（2）使用CH 2CO、卤代硫代甲醛和苯并吡喃硫酮等系统进行实验测试，（3）振动能流（IVR）的实验控制使用激光/分子相互作用和（4）对IVR进行建模。 实验将使用受激发射泵浦扩展分子束与超快泵浦/探测光谱进行。 理论工作将通过PI和其他人开发的MFD和SUR计算技术进行。这些研究将进一步了解振动能量如何通过受激发射或超快激光泵浦激发分子的扩展光束在复杂有机分子周围移动。 这将使用基于大规模从头计算RRKM的理论进行理论建模。 激光泵浦也将用于减缓能量转移的速率，从而启动控制化学反应的第一阶段。 这对光化学具有重要意义。

Martin Grubele of the University of Illinois at Urbana is supported by a grant from the Experimental Physical Chemistry Program to continue his work on vibrational energy flow in organic molecules. This involves (1) the extension of his theoretical models to include methanol, pyrrole, acetonitrile, ketene and thiophosgene, (2) experimental tests using systems such as CH2CO, halogenated thioformaldehydes and benzopyranthione, (3) experimental control of vibrational energy flow (IVR) using laser/molecule interactions and (4) modeling of IVR. The experiments will be carried out using stimulated emission pumping of expanding molecular beams with ultra fast pump/probe spectroscopy. The theoretical work will be carried out by MFD and SUR computational techniques developed by the PI and others.The studies will further understanding of how vibrational energy moves around complex organic molecules by exciting an expanding beam of molecules by stimulated emission or ultrafast laser pumping. This will be theoretically modeled using large scale ab initio RRKM based theory. The laser pumping will also be used to slow down the rate of energy transfer, thus initiating the first stage of controlling chemical reactions. This has important implications to photochemistry.