目前用于实时监测非共振强光驱动分子结构畸变、弛豫及运动状态的主要技术手段为离子成像技术、超快电子衍射与成像技术以及冲击受激光散射技术，但是他们具有各自的局限性：离子成像技术和超快电子衍射技术，仅能对高真空分子束中的孤立分子进行实时监测，而且离子成像技术在探测过程中平破坏了分子结构的完整性；而冲击受激光散射技术尽管无需高真空环境，适用于凝聚态分子取向弛豫过程的，但难以给出足够的分子的结构信息。本项目基于fs-CARS光谱技术，提出了“强泵浦时-频分辨CARS光谱技术”的新型技术方案，突破了上述技术的局限性，可用于固、液、气相的分子的研究，并可追踪分子振动结构演化及分子运动状态；通过操控和追踪几种凝聚相分子结构畸变与运动状态的实践，为分子学器件研究及化学反应微观机制的研究提供研究案例和技术支撑。

At present，the mainly used ultrafast technologies for real time monitoring molecular structure deformation, structure relaxation and motion driven by intense nonresonant laser pulse, are ion imaging, ultrafast electron diffration and imaging or impulsive stimulated light scattering. However their limitation are subsistent. For examples, ion imaging and ultafast electron diffraction and imaging only can be used for monitoring the isolated molecules in molecular beam in high vacuum chamber, and the molecular structure is destroyed in the process of ion imaging; impulsive stimulated light scattering can be used for real time monitoring reorientation processes of molecules in condensed phase, but it can not provide enough information of molecular structure. In this proposal, a novel ultrafast vibrational spectroscopy technology is proposed, named “intense pumping time-frequency CARS”， which break through the limitations of the technology mentioned above. The new technology is not only suitable for the research of molecules in gas liquid solid three phase, but also able to tracking the molecular structure deformation and motion. Several research cases of controlling and tracking molecular structure deformation and motion are proposed, which provide technical support for the researches of molecular devices and mechanisms of chemical reaction.