本项目系统的研究偏振整形飞秒脉冲序列作用下分子的准直优化及其激发态动力学过程的操控。将相干分子反应控制方法从一维推广到三维，实现更为有效的控制。项目将建立偏振整形飞秒激光的产生及其表征和校正方法。使用偏振态随时间可变的飞秒整形脉冲序列，产生三维空间准直的分子体系，提高分子体系准直程度。阐明不同的分子结构、不同的脉冲形状对应的准直机理。在前导脉冲序列已实现准直的分子体系上用后续不同偏振的脉冲或者偏振整形的脉冲序列控制三维分子的电离解离及异构化过程，控制与偏振相关的某个分子键的演化和断裂，实现对指定反应通道相对于非偏振整形激光更高程度的优化。并通过系统的改变脉冲参数或分析实验自优化结果阐明实现控制的机理。进一步将这些结果应用于激光成丝的研究中，使用偏振整形脉冲调控激光成丝传播过程中相关的分子准直过程及准直分子的激发态动力学过程，有效增加激光成丝传播距离、提高远距离气体成分探测灵敏度。

In this project, we propose a systematic study of molecule alignment and control of its excited state dynamics, by using polarization shaped femtosecond laser pulses. We extend the study of molecule reaction coherent control from one dimensional to three dimensional, to achieve more efficient control. In this project, we will develop the system of polarization shaped femtosecond laser pulse and its characterization and calibration methods. By using a shaped femtosecond laser pulse with its polarization change in time, we achieve three dimensional alignment of some model molecules, and higher degree of alignment, and to elucidate the effect of different molecular structure, pulse shape on the alignment process, to clarify the alignment mechanism. Next, we propose to control the ionization/dissociation and isomerization processes of the aligned molecules using subsequent different polarized pulses or polarization shaped pulses, to control the evolution and breaking of a polarization related bond, and to achieve higher degree of optimization over particular reaction channels, compared to non-polarization shaped laser, and to clarify the control mechanism by systematically varying pulse parameters or by analyzing the result from self-optimization. Furthermore, we will apply these results in the study of laser filamentation, we use polarization shaped femtosecond laser pulses to control related molecular alignment processes in the filament propagation and the excited state dynamics of aligned molecules, to effectively increase laser filament length and the sensitivity of remote molecule detection.