Infrared Laser control of molecular reaction dynamics in the electronic ground state. Theory and experiment

在这个项目中，我们研究了红外激光脉冲驱动的化学反应，通过特定的激发振动的电子基态，直接或通过能量弛豫途径连接到两个反应物之间的反应的反应坐标。我们将系统地激发高于和低于活化能的不同振动，并使用超快红外光谱实时跟踪瞬态动力学。IR激发下的动力学和产物形成提供了与化学反应和反应途径相关的反应坐标的基本信息。我们专注于醇和异氰酸酯反应物之间的醇解反应，产生氨基甲酸酯和聚氨酯产品。我们将巩固我们最近的红外脉冲驱动尿烷形成的结果，并研究同位素标记和改变振动激发能对醇解结果的影响。我们的研究将提供基本的洞察力，否则热驱动的反应在电子基态的反应途径。 这为能够产生复杂结构的IR激光引导的纳米聚合打开了可能性。

In this project, we investigate the IR laser pulse driven chemical reaction via specific excited vibrations in the electronic ground state, connected directly or via energy relaxation pathways to the reaction coordinate of the reaction between two reactants. We will excite systematically different vibrations above and below the activation energy and track the transient dynamics in real-time using ultrafast IR spectroscopy. The dynamics and product formation upon IR excitation provide essential information on the reaction coordinate related to the chemical reaction and the reaction pathway. We concentrate on the alcoholysis reaction between alcohol and isocyanate reactants yielding urethane and polyurethane products. We will consolidate our recent results on IR pulse driven urethane formation and investigate the impact of isotopic labelling and altered vibrational excitation energies on the outcome of alcoholysis. Our studies will provide fundamental insight into the reaction pathway of an otherwise thermally driven reactions in the electronic ground state. This opens the possibility for an IR laser guided nanopolymerization capable for creating complex structures.