RUI: Momentum Imaging Studies of Controlled Molecular Fragmentation

近年来，使用涉及整形激光脉冲的闭环方案控制了各种化学过程。然而，对于除了最基本的系统之外的所有系统，事实证明，要解构最佳的激光脉冲以恢复涉及激光-分子相互作用的分子动力学信息是具有挑战性的。另一方面，动量成像技术可以产生丰富的、相关的多维数据，这使得我们在理解许多光子和离子-分子相互作用方面取得了重大进展。这项建议中描述的研究计划将使用动量成像来探测由优化的激光脉冲引起的分子碎裂动力学。通过将能够将最佳脉冲形状归结为其本质特征的数值分析与动量成像提供的动力学的后验重建相结合，我们希望能推断出控制机制(S)。具体地说，PI建议使用闭环控制来识别用于选择性分子裂解的有趣的“最佳”脉冲，然后使用动量成像来研究由这些脉冲产生的控制机制。从成像测量中收集的信息也将用于探索定义最佳控制参数的多维表面的有趣拓扑。

A variety of chemical processes have been controlled in recent years using closed loop schemes involving shaped laser pulses. For all but the most basic systems, however, it has proved challenging to deconstruct the optimal laser pulse to recover information about the molecular dynamics involved in the laser-molecule interaction. On the other hand, momentum imaging techniques can produce rich, correlated, multi-dimensional data that has led to significant advances in our understanding of many photon- and ion-molecule interactions. The program of research described in this proposal would use momentum imaging to probe the molecular fragmentation dynamics arising from optimized laser pulses. By combining numerical analysis capable of reducing the optimal pulse shape to its essential features with a posteriori reconstruction of the dynamics afforded by momentum imaging, we hope to deduce the control mechanism(s). Specifically, the PI proposes to identify interesting "optimal" pulses for selective molecular fragmentation using closed-loop control and then use momentum imaging to investigate the control mechanisms produced by these pulses. Information gleaned from the imaging measurements will also be used to explore the interesting topology of the multidimensional surface that defines the optimal control parameters.