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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 Laboratory (SLAC), 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. https://doi.org/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. https://doi.org/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 = {Tue Apr 05 00:00:00 EDT 2016},
month = {Tue Apr 05 00:00:00 EDT 2016}
}

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Femtosecond Multidimensional Imaging of a Molecular Dissociation
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Time-Resolved Molecular Frame Dynamics of Fixed-in-Space CS2 Molecules
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Direct observation of the femtosecond excited-state cis-trans isomerization in bacteriorhodopsin
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Compression of sub-relativistic space-charge-dominated electron bunches for single-shot femtosecond electron diffraction
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Excited-state dynamics of molecules with classically driven trajectories and Gaussians
text, January 2019


Molecular movie of ultrafast coherent rotational dynamics of OCS
journal, July 2019

  • Karamatskos, Evangelos T.; Raabe, Sebastian; Mullins, Terry
  • Nature Communications, Vol. 10, Issue 1
  • DOI: 10.1038/s41467-019-11122-y

Time-dependent analysis of the mixed-field orientation of molecules without rotational symmetry
text, January 2017

  • Thesing, Linda V.; Küpper, Jochen; González-Férez, Rosario
  • Deutsches Elektronen-Synchrotron, DESY, Hamburg
  • DOI: 10.3204/pubdb-2017-07350

Excited-state dynamics of molecules with classically driven trajectories and Gaussians
text, January 2019


Time-dependent analysis of the mixed-field orientation of molecules without rotational symmetry
text, January 2017


Ultrafast Relativistic Electron Nanoprobes
text, January 2019


Probing ultrafast ππ*/nπ* internal conversion in organic chromophores via K-edge resonant absorption
journal, June 2017


A compact tunable quadrupole lens for brighter and sharper ultra-fast electron diffraction imaging
journal, March 2019


A novel nondestructive diagnostic method for mega-electron-volt ultrafast electron diffraction
journal, November 2019


A general method for baseline-removal in ultrafast electron powder diffraction data using the dual-tree complex wavelet transform
journal, December 2016

  • René de Cotret, Laurent P.; Siwick, Bradley J.
  • Structural Dynamics, Vol. 4, Issue 4
  • DOI: 10.1063/1.4972518

High current table-top setup for femtosecond gas electron diffraction
journal, July 2017

  • Zandi, Omid; Wilkin, Kyle J.; Xiong, Yanwei
  • Structural Dynamics, Vol. 4, Issue 4
  • DOI: 10.1063/1.4983225

Femtosecond gas-phase mega-electron-volt ultrafast electron diffraction
journal, September 2019

  • Shen, X.; Nunes, J. P. F.; Yang, J.
  • Structural Dynamics, Vol. 6, Issue 5
  • DOI: 10.1063/1.5120864

Molecular movie of ultrafast coherent rotational dynamics of OCS
text, January 2019

  • Karamatskos, Evangelos Thomas; Raabe, Sebastian; Mullins, Terence
  • Deutsches Elektronen-Synchrotron, DESY, Hamburg
  • DOI: 10.3204/pubdb-2019-02675