Abstract
We compare ultrafast electron and X-ray diffraction using quantum molecular dynamics simulations in photoexcited ethylene. The simulations of ethylene are done using the ab-initio multiconfigurational Ehrenfest (AI-MCE) approach, with electronic structure calculations at the SA3-CASSCF(2,2)/cc-ppVDZ level. The diffraction signal is calculated using the independent atom model. We find that the electron diffraction is more sensitive to the nuclear wavepacket, and the dynamics of the hydrogen atoms in particular.
Highlights
Ultrafast laser spectroscopy has developed dramatically over the past two decades, and constitutes today a large family of techniques capable of probing fundamental transformations of matter in astonishing detail [1,2]
Diffraction probes molecular geometry directly. This key advantage was recognised by Ahmed Zewail, who even before his 1999 Nobel Prize was working on ultrafast electron diffraction (UED) [3] and continued to pursue it vigorously after the Prize [4,5], in the footsteps of and alongside other pioneers [6,7,8]
This Letter, in recognition of Ahmed Zewail’s contributions to ultrafast spectroscopy, femtochemistry, and UED, compares the electron and X-ray diffraction signals predicted for the ultrafast dynamics of photoexcited ethylene using state-of-the-art quantum molecular dynamics simulations, with the aim of exploring the complementarities of ultrafast diffraction by either electrons or X-rays
Summary
Ultrafast laser spectroscopy has developed dramatically over the past two decades, and constitutes today a large family of techniques capable of probing fundamental transformations of matter in astonishing detail [1,2]. This key advantage was recognised by Ahmed Zewail, who even before his 1999 Nobel Prize was working on ultrafast electron diffraction (UED) [3] and continued to pursue it vigorously after the Prize [4,5], in the footsteps of and alongside other pioneers [6,7,8]. The introduction of high-energy electron beams overcame the space-charge and velocity mismatch problems that previously hampered the time-resolution of UED [22,23]. This brings us to the current and rather promising situation, where we have two powerful ultrafast diffraction techniques, one based on electrons and one on X-rays, both capable of complementing ultrafast spectroscopy. This Letter, in recognition of Ahmed Zewail’s contributions to ultrafast spectroscopy, femtochemistry, and UED, compares the electron and X-ray diffraction signals predicted for the ultrafast dynamics of photoexcited ethylene using state-of-the-art quantum molecular dynamics simulations, with the aim of exploring the complementarities of ultrafast diffraction by either electrons or X-rays
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