Scholarlink

<p>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.</p>

错误：搜索内容不能为空，请输入英文关键词
错误：关键词超出字数限制，请精简
高级检索

Super-resolution femtosecond electron diffraction reveals electronic and nuclear dynamics at conical intersections

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2025年7月21日

查看全文
  • Hui Jiang,
  • Juanjuan Zhang,
  • Tianyu Wang,
  • Jiawei Peng,
  • Cheng Jin,
  • Xiao Zou,
  • Pengfei Zhu,
  • Tao Jiang,
  • Zhenggang Lan,
  • Haiwang Yong,
  • Feng He,
  • Dao Xiang

摘要

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.