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

Fuente: arXiv
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Main Authors: Jiang, Hui, Zhang, Juanjuan, Wang, Tianyu, Peng, Jiawei, Jin, Cheng, Zou, Xiao, Zhu, Pengfei, Jiang, Tao, Lan, Zhenggang, Yong, Haiwang, FengHe, Xiang, Dao
Format: Preprint
Published: 2025
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author Jiang, Hui
Zhang, Juanjuan
Wang, Tianyu
Peng, Jiawei
Jin, Cheng
Zou, Xiao
Zhu, Pengfei
Jiang, Tao
Lan, Zhenggang
Yong, Haiwang
FengHe
Xiang, Dao
author_facet Jiang, Hui
Zhang, Juanjuan
Wang, Tianyu
Peng, Jiawei
Jin, Cheng
Zou, Xiao
Zhu, Pengfei
Jiang, Tao
Lan, Zhenggang
Yong, Haiwang
FengHe
Xiang, Dao
contents 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 angstrom 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.
format Preprint
id arxiv_https___arxiv_org_abs_2507_18948
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Super-resolution femtosecond electron diffraction reveals electronic and nuclear dynamics at conical intersections
Jiang, Hui
Zhang, Juanjuan
Wang, Tianyu
Peng, Jiawei
Jin, Cheng
Zou, Xiao
Zhu, Pengfei
Jiang, Tao
Lan, Zhenggang
Yong, Haiwang
FengHe
Xiang, Dao
Chemical Physics
Atomic and Molecular Clusters
Instrumentation and Detectors
Optics
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 angstrom 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.
title Super-resolution femtosecond electron diffraction reveals electronic and nuclear dynamics at conical intersections
topic Chemical Physics
Atomic and Molecular Clusters
Instrumentation and Detectors
Optics
url https://arxiv.org/abs/2507.18948