Jiang Hui, Zhang Juanjuan, Wang Tianyu, Peng Jiawei, Jin Cheng, Zou Xiao, Zhu Pengfei, Jiang Tao, Lan Zhenggang, Yong Haiwang, He Feng, Xiang Dao
Tsung-Dao Lee Institute, Shanghai Jiao Tong University, Shanghai, 201210, China.
Key Laboratory for Laser Plasmas (Ministry of Education) and School of Physics and Astronomy, Collaborative innovation center for IFSA (CICIFSA), Shanghai Jiao Tong University, Shanghai, 200240, China.
Nat Commun. 2025 Jul 21;16(1):6703. doi: 10.1038/s41467-025-61975-9.
Conical intersections play a pivotal role in excited-state quantum dynamics. Capturing transient molecular structures near conical intersections remains challenging due to the rapid timescales and subtle structural changes involved. We overcome this by combining the enhanced temporal resolution of mega-electron-volt ultrafast electron diffraction with a super-resolution real-space inversion algorithm, enabling visualization of nuclear and electronic motions at conical intersections with sub-angstrom resolution, surpassing the diffraction limit. We apply this technique to the textbook example of the ring-opening reaction of 1,3-cyclohexadiene, which proceeds through two conical intersections within 100 femtoseconds. The super-resolved transient structures near conical intersections reveal a C-C bond length difference of less than 0.4 Å and an approximately 30-femtosecond traversal time of the nuclear wave packet between them. These findings establish super-resolution ultrafast scattering as a transformative tool for uncovering quantum dynamics in molecules and open new avenues for studying light-matter interactions at the most fundamental level.
锥形交叉点在激发态量子动力学中起着关键作用。由于涉及快速的时间尺度和微妙的结构变化，捕获锥形交叉点附近的瞬态分子结构仍然具有挑战性。我们通过将兆电子伏特超快电子衍射的增强时间分辨率与超分辨率实空间反演算法相结合来克服这一问题，从而能够以亚埃分辨率可视化锥形交叉点处的核运动和电子运动，超越了衍射极限。我们将这项技术应用于1,3 - 环己二烯开环反应这个教科书式的例子，该反应在100飞秒内通过两个锥形交叉点进行。锥形交叉点附近的超分辨瞬态结构显示出碳 - 碳键长差异小于0.4 Å，并且核波包在它们之间的穿越时间约为30飞秒。这些发现确立了超分辨率超快散射作为揭示分子中量子动力学的变革性工具，并为在最基本层面研究光与物质相互作用开辟了新途径。
