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

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. Lastly, our results demonstrate a significant and promising step towards making atomically resolved movies of molecular reactions.

Authors:
 [1];  [2];  [3]; ORCiD logo [1];  [3];  [3];  [3];  [3];  [3];  [3];  [3];  [3];  [3];  [3];  [3];  [3];  [3];  [3];  [3];  [3] more »; ORCiD logo [3];  [1];  [3] « less
  1. Univ. of Nebraska-Lincoln, Lincoln, NE (United States)
  2. SLAC National Accelerator Lab., Menlo Park, CA (United States); Potsdam Univ., Potsdam (Germany)
  3. SLAC National Accelerator Lab., Menlo Park, CA (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1251412
Alternate Identifier(s):
OSTI ID: 1335955
Grant/Contract Number:  
AC02-76SF00515
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 7; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND TECHNOLOGY; chemical sciences; optical sciences; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 73 NUCLEAR PHYSICS AND RADIATION PHYSICS

Citation Formats

Yang, Jie, Guehr, Markus, Vecchione, Theodore, Robinson, Matthew S., Li, Renkai, Hartmann, Nick, Shen, Xiaozhe, Coffee, Ryan, Corbett, Jeff, Fry, Alan, Gaffney, Kelly, Gorkhover, Tais, Hast, Carsten, Jobe, Keith, Makasyuk, Igor, Reid, Alexander, Robinson, Joseph, Vetter, Sharon, Wang, Fenglin, Weathersby, Stephen, Yoneda, Charles, Centurion, Martin, and Wang, Xijie. Diffractive imaging of a rotational wavepacket in nitrogen molecules with femtosecond megaelectronvolt electron pulses. United States: N. p., 2016. Web. doi:10.1038/ncomms11232.
Yang, Jie, Guehr, Markus, Vecchione, Theodore, Robinson, Matthew S., Li, Renkai, Hartmann, Nick, Shen, Xiaozhe, Coffee, Ryan, Corbett, Jeff, Fry, Alan, Gaffney, Kelly, Gorkhover, Tais, Hast, Carsten, Jobe, Keith, Makasyuk, Igor, Reid, Alexander, Robinson, Joseph, Vetter, Sharon, Wang, Fenglin, Weathersby, Stephen, Yoneda, Charles, Centurion, Martin, & Wang, Xijie. Diffractive imaging of a rotational wavepacket in nitrogen molecules with femtosecond megaelectronvolt electron pulses. United States. doi:10.1038/ncomms11232.
Yang, Jie, Guehr, Markus, Vecchione, Theodore, Robinson, Matthew S., Li, Renkai, Hartmann, Nick, Shen, Xiaozhe, Coffee, Ryan, Corbett, Jeff, Fry, Alan, Gaffney, Kelly, Gorkhover, Tais, Hast, Carsten, Jobe, Keith, Makasyuk, Igor, Reid, Alexander, Robinson, Joseph, Vetter, Sharon, Wang, Fenglin, Weathersby, Stephen, Yoneda, Charles, Centurion, Martin, and Wang, Xijie. Tue . "Diffractive imaging of a rotational wavepacket in nitrogen molecules with femtosecond megaelectronvolt electron pulses". United States. doi:10.1038/ncomms11232. https://www.osti.gov/servlets/purl/1251412.
@article{osti_1251412,
title = {Diffractive imaging of a rotational wavepacket in nitrogen molecules with femtosecond megaelectronvolt electron pulses},
author = {Yang, Jie and Guehr, Markus and Vecchione, Theodore and Robinson, Matthew S. and Li, Renkai and Hartmann, Nick and Shen, Xiaozhe and Coffee, Ryan and Corbett, Jeff and Fry, Alan and Gaffney, Kelly and Gorkhover, Tais and Hast, Carsten and Jobe, Keith and Makasyuk, Igor and Reid, Alexander and Robinson, Joseph and Vetter, Sharon and Wang, Fenglin and Weathersby, Stephen and Yoneda, Charles and Centurion, Martin and Wang, Xijie},
abstractNote = {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. Lastly, our results demonstrate a significant and promising step towards making atomically resolved movies of molecular reactions.},
doi = {10.1038/ncomms11232},
journal = {Nature Communications},
number = ,
volume = 7,
place = {United States},
year = {2016},
month = {4}
}

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