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Diffractive imaging of a rotational wavepacket in nitrogen molecules with femtosecond megaelectronvolt electron pulses

Author

Listed:
  • Jie Yang

    (University of Nebraska-Lincoln)

  • Markus Guehr

    (PULSE Institute, SLAC National Accelerator Laboratory
    Institute of Physics and Astronomy, Potsdam University)

  • Theodore Vecchione

    (SLAC National Accelerator Laboratory)

  • Matthew S. Robinson

    (University of Nebraska-Lincoln)

  • Renkai Li

    (SLAC National Accelerator Laboratory)

  • Nick Hartmann

    (SLAC National Accelerator Laboratory)

  • Xiaozhe Shen

    (SLAC National Accelerator Laboratory)

  • Ryan Coffee

    (SLAC National Accelerator Laboratory)

  • Jeff Corbett

    (SLAC National Accelerator Laboratory)

  • Alan Fry

    (SLAC National Accelerator Laboratory)

  • Kelly Gaffney

    (SLAC National Accelerator Laboratory)

  • Tais Gorkhover

    (SLAC National Accelerator Laboratory)

  • Carsten Hast

    (SLAC National Accelerator Laboratory)

  • Keith Jobe

    (SLAC National Accelerator Laboratory)

  • Igor Makasyuk

    (SLAC National Accelerator Laboratory)

  • Alexander Reid

    (SLAC National Accelerator Laboratory)

  • Joseph Robinson

    (SLAC National Accelerator Laboratory)

  • Sharon Vetter

    (SLAC National Accelerator Laboratory)

  • Fenglin Wang

    (SLAC National Accelerator Laboratory)

  • Stephen Weathersby

    (SLAC National Accelerator Laboratory)

  • Charles Yoneda

    (SLAC National Accelerator Laboratory)

  • Martin Centurion

    (University of Nebraska-Lincoln)

  • Xijie Wang

    (SLAC National Accelerator Laboratory)

Abstract

Imaging changes in molecular geometries on their natural femtosecond timescale with sub-Angström spatial precision is one of the critical challenges in the chemical sciences, as the nuclear geometry changes determine the molecular reactivity. For photoexcited molecules, the nuclear dynamics determine the photoenergy conversion path and efficiency. Here we report a gas-phase electron diffraction experiment using megaelectronvolt (MeV) electrons, where we captured the rotational wavepacket dynamics of nonadiabatically laser-aligned nitrogen molecules. We achieved a combination of 100 fs root-mean-squared temporal resolution and sub-Angstrom (0.76 Å) spatial resolution that makes it possible to resolve the position of the nuclei within the molecule. In addition, the diffraction patterns reveal the angular distribution of the molecules, which changes from prolate (aligned) to oblate (anti-aligned) in 300 fs. Our results demonstrate a significant and promising step towards making atomically resolved movies of molecular reactions.

Suggested Citation

  • Jie Yang & Markus Guehr & Theodore Vecchione & Matthew S. Robinson & Renkai Li & Nick Hartmann & Xiaozhe Shen & Ryan Coffee & Jeff Corbett & Alan Fry & Kelly Gaffney & Tais Gorkhover & Carsten Hast & , 2016. "Diffractive imaging of a rotational wavepacket in nitrogen molecules with femtosecond megaelectronvolt electron pulses," Nature Communications, Nature, vol. 7(1), pages 1-9, September.
    • Handle: RePEc:nat:natcom:v:7:y:2016:i:1:d:10.1038_ncomms11232
    DOI: 10.1038/ncomms11232
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    Cited by:

    1. Terry Mullins & Evangelos T. Karamatskos & Joss Wiese & Jolijn Onvlee & Arnaud Rouzée & Andrey Yachmenev & Sebastian Trippel & Jochen Küpper, 2022. "Picosecond pulse-shaping for strong three-dimensional field-free alignment of generic asymmetric-top molecules," Nature Communications, Nature, vol. 13(1), pages 1-7, December.

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