Tang Zilong, Jarupula Ramesh, Yong Haiwang
Department of Chemistry and Biochemistry, University of California, San Diego, La Jolla, CA 92093, USA.
Program in Materials Science and Engineering, University of California, San Diego, La Jolla, CA 92093, USA.
iScience. 2024 Aug 10;27(9):110705. doi: 10.1016/j.isci.2024.110705. eCollection 2024 Sep 20.
Quantum coherence governs the outcome and efficiency of photochemical reactions and ultrafast molecular dynamics. Recent ultrafast gas-phase X-ray scattering and electron diffraction have enabled the observation of femtosecond nuclear dynamics driven by vibrational coherence. However, probing attosecond electron dynamics and coupled electron-nuclear dynamics remains challenging. This article discusses advances in ultrafast X-ray scattering and electron diffraction, highlighting their potential to resolve attosecond charge migration and vibronic coupling at conical intersections. Novel techniques, such as X-ray scattering with orbital angular momentum beams and combined X-ray and electron diffraction, promise to selectively probe coherence contributions and visualize charge migration in real-space. These emerging methods could further our understanding of coherence effects in chemical reactions.
量子相干控制着光化学反应和超快分子动力学的结果与效率。近期的超快气相X射线散射和电子衍射使得对由振动相干驱动的飞秒核动力学的观测成为可能。然而,探测阿秒电子动力学以及耦合的电子-核动力学仍然具有挑战性。本文讨论了超快X射线散射和电子衍射的进展,突出了它们在锥形交叉点解析阿秒电荷迁移和振子耦合的潜力。诸如利用轨道角动量光束进行X射线散射以及联合X射线和电子衍射等新技术,有望选择性地探测相干贡献并在实空间中可视化电荷迁移。这些新兴方法能够增进我们对化学反应中相干效应的理解。