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

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

doi:10.1038/ncomms11232

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

Journal Article · Tue Apr 05 00:00:00 EDT 2016 · Nature Communications

DOI:https://doi.org/10.1038/ncomms11232· OSTI ID:1251412

Yang, Jie ^[1]; Guehr, Markus ^[2]; Vecchione, Theodore ^[3];

^[1]; Li, Renkai ^[3]; Hartmann, Nick ^[3]; Shen, Xiaozhe ^[3]; Coffee, Ryan ^[3]; Corbett, Jeff ^[3]; Fry, Alan ^[3]; Gaffney, Kelly ^[3]; Gorkhover, Tais ^[3]; Hast, Carsten ^[3]; Jobe, Keith ^[3]; Makasyuk, Igor ^[3]; Reid, Alexander ^[3]; Robinson, Joseph ^[3]; Vetter, Sharon ^[3]; Wang, Fenglin ^[3]; Weathersby, Stephen ^[3] more »

Univ. of Nebraska-Lincoln, Lincoln, NE (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States); Potsdam Univ., Potsdam (Germany)
SLAC National Accelerator Lab., Menlo Park, CA (United States)

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.

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

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 1251412

Alternate ID(s):: OSTI ID: 1335955

Journal Information:: Nature Communications, Vol. 7; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 78 works

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X-ray diffractive imaging of controlled gas-phase molecules: Toward imaging of dynamics in the molecular frame Kierspel, Thomas; Morgan, Andrew; Wiese, Joss Deutsches Elektronen-Synchrotron, DESY, Hamburg https://doi.org/10.3204/pubdb-2020-00943	text	January 2020
Excited-state dynamics of molecules with classically driven trajectories and Gaussians Ibele, Lea M.; Nicolson, Angus; Curchod, Basile F. E. Taylor & Francis https://doi.org/10.6084/m9.figshare.9912614.v1	text	January 2019
Molecular movie of ultrafast coherent rotational dynamics of OCS Karamatskos, Evangelos T.; Raabe, Sebastian; Mullins, Terry Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-11122-y	journal	July 2019
Time-dependent analysis of the mixed-field orientation of molecules without rotational symmetry Thesing, Linda V.; Küpper, Jochen; González-Férez, Rosario Deutsches Elektronen-Synchrotron, DESY, Hamburg https://doi.org/10.3204/pubdb-2017-07350	text	January 2017
Excited-state dynamics of molecules with classically driven trajectories and Gaussians Ibele, Lea M.; Nicolson, Angus; Curchod, Basile F. E. Taylor & Francis https://doi.org/10.6084/m9.figshare.9912614	text	January 2019
Time-dependent analysis of the mixed-field orientation of molecules without rotational symmetry Thesing, Linda V.; Küpper, Jochen; González-Férez, Rosario arXiv https://doi.org/10.48550/arxiv.1705.03225	text	January 2017
Attomicroscopy: from Femtosecond to Attosecond Electron Microscopy Hassan, Mohammed Th. arXiv https://doi.org/10.48550/arxiv.1801.04350	text	January 2018
RichMol: A general variational approach for rovibrational molecular dynamics in external electric fields Owens, Alec; Yachmenev, Andrey arXiv https://doi.org/10.48550/arxiv.1802.07603	text	January 2018
Ultrafast Relativistic Electron Nanoprobes Ji, Fu-Hao; Durham, Daniel; Minor, Andrew arXiv https://doi.org/10.48550/arxiv.1901.03443	text	January 2019
Femtosecond compression dynamics and timing jitter suppression in a terahertz-driven electron bunch compressor Snively, E. C.; Othman, M. A. K.; Kozina, M. arXiv https://doi.org/10.48550/arxiv.1906.03358	text	January 2019
A compact tunable quadrupole lens for brighter and sharper ultra-fast electron diffraction imaging Yang, Xi; Yu, Lihua; Smaluk, Victor Scientific Reports, Vol. 9, Issue 1 https://doi.org/10.1038/s41598-019-39208-z	journal	March 2019
A general method for baseline-removal in ultrafast electron powder diffraction data using the dual-tree complex wavelet transform René de Cotret, Laurent P.; Siwick, Bradley J. Structural Dynamics, Vol. 4, Issue 4 https://doi.org/10.1063/1.4972518	journal	December 2016

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