高时空分辨的分子轨道成像是深入研究物质微观世界的重要手段，对于物理学、化学、乃至材料科学与生命科学都有着举足轻重的作用，一直以来是国内外研究的前沿热点。近年来，人们发现通过分子在强光场中的高次谐波辐射和电离过程可以获得埃空间尺度和飞秒时间尺度的分子轨道演化信息，从而实现高时空分辨的分子轨道成像。目前在分子轨道高时空分辨成像及其相关关键科学问题的研究中，主要是通过测量不同排列角度的分子在强光场中的高次谐波信号或者光电子信号来获取分子轨道的全方位信息，而预排列脉冲带来的轨道畸变以及多次测量带来的误差是造成成像分辨率及精度不高的重要原因。本项目提出采用非平行偏振双色光场开展分子轨道成像的研究，通过精密操纵分子轨道电离以及连续态电子波包动力学过程,在单个脉冲与分子相互作用过程中获取分子轨道的全方位信息，发展相关重构算法，最终实现分子轨道高分辨率、高精度的单发成像。

Molecular orbital imaging methods with high spatio-temporal resolutions are important tools for the investigations of the microscopic world, which are critical for the progress in physics, chemistry, materials science and life sciences, and have attracted a lot of attentions around the world. In the near ten years, it has been found that one can extract the information about the molecular orbitals with femtosecond-temporal and angstrom-spatial resolutions via the strong field processes such as the high-order harmonic generation (HHG) and strong field ionizations, which paves the way to the imaging methods with extremely high spatio-temporal resolution. In the current research of the molecular orbital imaging and the corresponding scientific issues, the overall information of the objective molecular orbital is obtained from the HHG or photoelectron signals after the molecule is aligned in various directions. However, the deformation of the orbital by the pre-alignment pulses and the errors associated with the multiple-shot detection will lead to the low accuracy and resolution. In this project, we propose a new imaging method with non-colinearly polarized tow-color optical fields. By quamtum manipulations of the ionization of the molecular orbital and the dynamics of the continuum electrons, it is possible to extract the overall information of the molecular orbital after the interaction of the molecule with only one pulse. We are going to develop the reconstruction algorithm, and finally achieve the one-shot molecular orbital imaging with high spatio-temporal resolutions.