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

Champenois, Elio G.; List, Nanna H.; Ware, Matthew; Britton, Mathew; Bucksbaum, Philip H.; Cheng, Xinxin; Centurion, Martin; Cryan, James P.; Forbes, Ruaridh; Gabalski, Ian; Hegazy, Kareem; Hoffmann, Matthias C.; Howard, Andrew J.; Ji, Fuhao; Lin, Ming-Fu; Nunes, J. Pedro F.; Shen, Xiaozhe; Yang, Jie; Wang, Xijie; Martinez, Todd J.; Wolf, Thomas J. A.

doi:10.1103/physrevlett.131.143001

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

Journal Article · Thu Oct 05 00:00:00 EDT 2023 · Physical Review Letters

DOI:https://doi.org/10.1103/physrevlett.131.143001· OSTI ID:2439986

Champenois, Elio G. ^[1]; ^[2]; Ware, Matthew ^[3]; Britton, Mathew ^[4]; ^[4]; ^[5]; ^[6]; ^[3]; ^[5]; Gabalski, Ian ^[4]; ^[4]; Hoffmann, Matthias C. ^[5]; Howard, Andrew J. ^[4]; Ji, Fuhao ^[5]; ^[5]; ^[6]; Shen, Xiaozhe ^[5]; Yang, Jie ^[7]; ^[5]; ^[4] more »

SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Institute (PULSE); SLAC
KTH Royal Inst. of Technology, Stockholm (Sweden)
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Institute (PULSE)
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Institute (PULSE); Stanford Univ., CA (United States)
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Univ. of Nebraska, Lincoln, NE (United States)
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Tsinghua Univ., Beijing (China)

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 here represent an important step towards the observation of proton dynamics in real space and time.

View Accepted Manuscript (DOE)

Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC02-05CH11231; AC02-76SF00515; SC0014170

OSTI ID:: 2439986

Journal Information:: Physical Review Letters, Journal Name: Physical Review Letters Journal Issue: 14 Vol. 131; ISSN 0031-9007

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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

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