skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Diffractive Imaging of Coherent Nuclear Motion in Isolated Molecules

Abstract

Observing the motion of the nuclear wave packets during a molecular reaction, in both space and time, is crucial for understanding and controlling the outcome of photoinduced chemical reactions. We have imaged the motion of a vibrational wave packet in isolated iodine molecules using ultrafast electron diffraction with relativistic electrons. The time-varying interatomic distance was measured with a precision 0.07 Å and temporal resolution of 230 fs full width at half maximum. The method is not only sensitive to the position but also the shape of the nuclear wave packet.

Authors:
; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1335104
Report Number(s):
SLAC-PUB-16860
Journal ID: ISSN 0031-9007; PRLTAO; arXiv:1608.07725
DOE Contract Number:  
AC02-76SF00515
Resource Type:
Journal Article
Journal Name:
Physical Review Letters
Additional Journal Information:
Journal Volume: 117; Journal Issue: 15; Journal ID: ISSN 0031-9007
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
73 NUCLEAR PHYSICS AND RADIATION PHYSICS; ACCPHY

Citation Formats

Yang, Jie, Guehr, Markus, Shen, Xiaozhe, Li, Renkai, Vecchione, Theodore, Coffee, Ryan, Corbett, Jeff, Fry, Alan, Hartmann, Nick, Hast, Carsten, Hegazy, Kareem, Jobe, Keith, Makasyuk, Igor, Robinson, Joseph, Robinson, Matthew S., Vetter, Sharon, Weathersby, Stephen, Yoneda, Charles, Wang, Xijie, and Centurion, Martin. Diffractive Imaging of Coherent Nuclear Motion in Isolated Molecules. United States: N. p., 2016. Web. doi:10.1103/PhysRevLett.117.153002.
Yang, Jie, Guehr, Markus, Shen, Xiaozhe, Li, Renkai, Vecchione, Theodore, Coffee, Ryan, Corbett, Jeff, Fry, Alan, Hartmann, Nick, Hast, Carsten, Hegazy, Kareem, Jobe, Keith, Makasyuk, Igor, Robinson, Joseph, Robinson, Matthew S., Vetter, Sharon, Weathersby, Stephen, Yoneda, Charles, Wang, Xijie, & Centurion, Martin. Diffractive Imaging of Coherent Nuclear Motion in Isolated Molecules. United States. doi:10.1103/PhysRevLett.117.153002.
Yang, Jie, Guehr, Markus, Shen, Xiaozhe, Li, Renkai, Vecchione, Theodore, Coffee, Ryan, Corbett, Jeff, Fry, Alan, Hartmann, Nick, Hast, Carsten, Hegazy, Kareem, Jobe, Keith, Makasyuk, Igor, Robinson, Joseph, Robinson, Matthew S., Vetter, Sharon, Weathersby, Stephen, Yoneda, Charles, Wang, Xijie, and Centurion, Martin. Mon . "Diffractive Imaging of Coherent Nuclear Motion in Isolated Molecules". United States. doi:10.1103/PhysRevLett.117.153002. https://www.osti.gov/servlets/purl/1335104.
@article{osti_1335104,
title = {Diffractive Imaging of Coherent Nuclear Motion in Isolated Molecules},
author = {Yang, Jie and Guehr, Markus and Shen, Xiaozhe and Li, Renkai and Vecchione, Theodore and Coffee, Ryan and Corbett, Jeff and Fry, Alan and Hartmann, Nick and Hast, Carsten and Hegazy, Kareem and Jobe, Keith and Makasyuk, Igor and Robinson, Joseph and Robinson, Matthew S. and Vetter, Sharon and Weathersby, Stephen and Yoneda, Charles and Wang, Xijie and Centurion, Martin},
abstractNote = {Observing the motion of the nuclear wave packets during a molecular reaction, in both space and time, is crucial for understanding and controlling the outcome of photoinduced chemical reactions. We have imaged the motion of a vibrational wave packet in isolated iodine molecules using ultrafast electron diffraction with relativistic electrons. The time-varying interatomic distance was measured with a precision 0.07 Å and temporal resolution of 230 fs full width at half maximum. The method is not only sensitive to the position but also the shape of the nuclear wave packet.},
doi = {10.1103/PhysRevLett.117.153002},
journal = {Physical Review Letters},
issn = {0031-9007},
number = 15,
volume = 117,
place = {United States},
year = {2016},
month = {10}
}

Works referenced in this record:

Mapping molecular motions leading to charge delocalization with ultrabright electrons
journal, April 2013

  • Gao, Meng; Lu, Cheng; Jean-Ruel, Hubert
  • Nature, Vol. 496, Issue 7445
  • DOI: 10.1038/nature12044

Direct observation of collective modes coupled to molecular orbital-driven charge transfer
journal, December 2015


Direct Imaging of Transient Molecular Structures with Ultrafast Diffraction
journal, January 2001


Dark Structures in Molecular Radiationless Transitions Determined by Ultrafast Diffraction
journal, January 2005


Ultrafast diffraction and structural dynamics: The nature of complex molecules far from equilibrium
journal, June 2001

  • Ruan, C. -Y.; Lobastov, V. A.; Srinivasan, R.
  • Proceedings of the National Academy of Sciences, Vol. 98, Issue 13
  • DOI: 10.1073/pnas.131192898

Imaging of Isolated Molecules with Ultrafast Electron Pulses
journal, September 2012


Imaging of alignment and structural changes of carbon disulfide molecules using ultrafast electron diffraction
journal, September 2015

  • Yang, Jie; Beck, Joshua; Uiterwaal, Cornelis J.
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms9172

The Validity of the "Diradical" Hypothesis: Direct Femtoscond Studies of the Transition-State Structures
journal, November 1994


Direct observation of the femtosecond excited-state cis-trans isomerization in bacteriorhodopsin
journal, May 1988


Time-Resolved Molecular Frame Dynamics of Fixed-in-Space CS2 Molecules
journal, March 2009


The Ultrafast Pathway of Photon-Induced Electrocyclic Ring-Opening Reactions: The Case of 1,3-Cyclohexadiene
journal, May 2011


Imaging Molecular Motion: Femtosecond X-Ray Scattering of an Electrocyclic Chemical Reaction
journal, June 2015


Imaging ultrafast molecular dynamics with laser-induced electron diffraction
journal, March 2012

  • Blaga, Cosmin I.; Xu, Junliang; DiChiara, Anthony D.
  • Nature, Vol. 483, Issue 7388
  • DOI: 10.1038/nature10820

Imaging an aligned polyatomic molecule with laser-induced electron diffraction
journal, June 2015

  • Pullen, Michael G.; Wolter, Benjamin; Le, Anh-Thu
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms8262

Experimental observation of high-brightness microbunching in a photocathode rf electron gun
journal, October 1996


Femto-seconds electron beam diffraction using photocathode RF gun
conference, January 2003

  • Wang, X. J.; Wu, Z.; Ihee, H. H.
  • 2003 Particle Accelerator Conference, Proceedings of the 2003 Bipolar/BiCMOS Circuits and Technology Meeting (IEEE Cat. No.03CH37440)
  • DOI: 10.1109/PAC.2003.1288940

Ultrafast time-resolved electron diffraction with megavolt electron beams
journal, October 2006

  • Hastings, J. B.; Rudakov, F. M.; Dowell, D. H.
  • Applied Physics Letters, Vol. 89, Issue 18
  • DOI: 10.1063/1.2372697

Mega-electron-volt ultrafast electron diffraction at SLAC National Accelerator Laboratory
journal, July 2015

  • Weathersby, S. P.; Brown, G.; Centurion, M.
  • Review of Scientific Instruments, Vol. 86, Issue 7
  • DOI: 10.1063/1.4926994

Mapping atomic motions with ultrabright electrons: towards fundamental limits in space-time resolution
journal, January 2015

  • Manz, Stephanie; Casandruc, Albert; Zhang, Dongfang
  • Faraday Discussions, Vol. 177
  • DOI: 10.1039/C4FD00204K

Diffractive imaging of a rotational wavepacket in nitrogen molecules with femtosecond megaelectronvolt electron pulses
journal, April 2016

  • Yang, Jie; Guehr, Markus; Vecchione, Theodore
  • Nature Communications, Vol. 7, Issue 1
  • DOI: 10.1038/ncomms11232

Reconstruction of three-dimensional molecular structure from diffraction of laser-aligned molecules
journal, July 2014

  • Yang, Jie; Makhija, Varun; Kumarappan, Vinod
  • Structural Dynamics, Vol. 1, Issue 4
  • DOI: 10.1063/1.4889840

Reinvestigation of the Molecular Structure of 1,3,5,7‐Cyclooctatetraene by Electron Diffraction
journal, December 1957

  • Bastiansen, O.; Hedberg, Lise; Hedberg, Kenneth
  • The Journal of Chemical Physics, Vol. 27, Issue 6
  • DOI: 10.1063/1.1743999

Erratum : Reinvestigation of the Molecular Structure of 1,3,5,7‐Cyclooctatetraene
journal, March 1958

  • Bastiansen, O.; Hedberg, Lise; Hedberg, Kenneth
  • The Journal of Chemical Physics, Vol. 28, Issue 3
  • DOI: 10.1063/1.1744173

elsepa—Dirac partial-wave calculation of elastic scattering of electrons and positrons by atoms, positive ions and molecules
journal, January 2005

  • Salvat, Francesc; Jablonski, Aleksander; Powell, Cedric J.
  • Computer Physics Communications, Vol. 165, Issue 2
  • DOI: 10.1016/j.cpc.2004.09.006

Ultrafast Electron Diffraction (UED): A New Development for the 4D Determination of Transient Molecular Structures
journal, June 2003

  • Srinivasan, Ramesh; Lobastov, Vladimir A.; Ruan, Chong-Yu
  • Helvetica Chimica Acta, Vol. 86, Issue 6
  • DOI: 10.1002/hlca.200390147

Time-Resolved Electron Diffraction from Selectively Aligned Molecules
journal, May 2009


Pump–probe diffraction imaging of vibrational wave functions
journal, May 1998

  • Geiser, Joseph D.; Weber, Peter M.
  • The Journal of Chemical Physics, Vol. 108, Issue 19
  • DOI: 10.1063/1.476239

Mechanism and Dynamics of Azobenzene Photoisomerization
journal, July 2003

  • Schultz, Thomas; Quenneville, Jason; Levine, Benjamin
  • Journal of the American Chemical Society, Vol. 125, Issue 27
  • DOI: 10.1021/ja021363x

Time-resolved imaging of purely valence-electron dynamics during a chemical reaction
journal, April 2011

  • Hockett, Paul; Bisgaard, Christer Z.; Clarkin, Owen J.
  • Nature Physics, Vol. 7, Issue 8
  • DOI: 10.1038/nphys1980

Time-Resolved Photoelectron Spectra of CS 2 : Dynamics at Conical Intersections
journal, March 2014


Compression of Subrelativistic Space-Charge-Dominated Electron Bunches for Single-Shot Femtosecond Electron Diffraction
journal, December 2010


Imaging single electrons to enable the generation of ultrashort beams for single-shot femtosecond relativistic electron diffraction
journal, October 2011

  • Li, R. K.; Musumeci, P.; Bender, H. A.
  • Journal of Applied Physics, Vol. 110, Issue 7
  • DOI: 10.1063/1.3646465

Single shot time stamping of ultrabright radio frequency compressed electron pulses
journal, July 2013

  • Gao, M.; Jiang, Y.; Kassier, G. H.
  • Applied Physics Letters, Vol. 103, Issue 3
  • DOI: 10.1063/1.4813313

Self-Referenced Coherent Diffraction X-Ray Movie of Ångstrom- and Femtosecond-Scale Atomic Motion
journal, October 2016


    Works referencing / citing this record:

    Atomic-resolution imaging of carbonyl sulfide by laser-induced electron diffraction
    journal, June 2019

    • Karamatskos, Evangelos T.; Goldsztejn, Gildas; Raabe, Sebastian
    • The Journal of Chemical Physics, Vol. 150, Issue 24
    • DOI: 10.1063/1.5093959

    Time-resolved inner-shell photoelectron spectroscopy: From a bound molecule to an isolated atom
    journal, April 2018


    Ultrashort Free-Electron Laser X-ray Pulses
    journal, September 2017

    • Helml, Wolfram; Grguraš, Ivanka; Juranić, Pavle
    • Applied Sciences, Vol. 7, Issue 9
    • DOI: 10.3390/app7090915

    Ultrafast X-ray scattering reveals vibrational coherence following Rydberg excitation
    journal, July 2019