Femtosecond Electronic and Hydrogen Structural Dynamics in Ammonia Imaged with Ultrafast Electron Diffraction

被引：15
作者：
Champenois E.G. [1 ,4 ]
List N.H. [2 ]
Ware M. [1 ,4 ]
Britton M. [1 ,3 ,4 ]
Bucksbaum P.H. [1 ,3 ,4 ]
Cheng X. [4 ]
Centurion M. [5 ]
Cryan J.P. [1 ,4 ]
Forbes R. [4 ]
Gabalski I. [1 ,4 ,6 ]
Hegazy K. [1 ,3 ,4 ]
Hoffmann M.C. [4 ]
Howard A.J. [1 ,4 ,6 ]
Ji F. [4 ]
Lin M.-F. [4 ]
Nunes J.P.F. [5 ]
Shen X. [4 ]
Yang J. [4 ,7 ]
Wang X. [4 ]
Martinez T.J. [1 ,4 ,8 ]
Wolf T.J.A. [1 ,4 ]
机构：
[1] Stanford Pulse Institute, Slac National Accelerator Laboratory, Menlo Park, 94025, CA
[2] Department of Chemistry, Kth Royal Institute of Technology, Stockholm
[3] Department of Physics, Stanford University, Stanford, 94305, CA
[4] Slac National Accelerator Laboratory, Menlo Park, 94025, CA
[5] Department of Physics and Astronomy, University of Nebraska Lincoln, Lincoln, 68588, NE
[6] Department of Applied Physics, Stanford University, Stanford, 94305, CA
[7] Department of Chemistry, Tsinghua University, Beijing
[8] Department of Chemistry, Stanford University, Stanford, 94305, CA
来源：
Physical Review Letters | 2023年 / 131卷 / 14期
关键词：
Compendex;
D O I：
10.1103/PhysRevLett.131.143001
中图分类号：
学科分类号：
摘要：
Directly imaging structural dynamics involving hydrogen atoms by ultrafast diffraction methods is complicated by their low scattering cross sections. Here we demonstrate that megaelectronvolt ultrafast electron diffraction is sufficiently sensitive to follow hydrogen dynamics in isolated molecules. In a study of the photodissociation of gas phase ammonia, we simultaneously observe signatures of the nuclear and corresponding electronic structure changes resulting from the dissociation dynamics in the time-dependent diffraction. Both assignments are confirmed by ab initio simulations of the photochemical dynamics and the resulting diffraction observable. While the temporal resolution of the experiment is insufficient to resolve the dissociation in time, our results represent an important step towards the observation of proton dynamics in real space and time. © 2023 American Physical Society.
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