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Title: Liquid-phase mega-electron-volt ultrafast electron diffraction

Abstract

The conversion of light into usable chemical and mechanical energy is pivotal to several biological and chemical processes, many of which occur in solution. To understand the structure–function relationships mediating these processes, a technique with high spatial and temporal resolutions is required. Here, we report on the design and commissioning of a liquid-phase mega-electron-volt (MeV) ultrafast electron diffraction instrument for the study of structural dynamics in solution. Limitations posed by the shallow penetration depth of electrons and the resulting information loss due to multiple scattering and the technical challenge of delivering liquids to vacuum were overcome through the use of MeV electrons and a gas-accelerated thin liquid sheet jet. To demonstrate the capabilities of this instrument, the structure of water and its network were resolved up to the 3rd hydration shell with a spatial resolution of 0.6 Å; preliminary time-resolved experiments demonstrated a temporal resolution of 200 fs.

Authors:
ORCiD logo [1]; ORCiD logo [2];  [3]; ORCiD logo [3];  [3];  [4];  [5];  [6];  [3];  [3];  [3];  [7]; ORCiD logo [3];  [3];  [3];  [3];  [3]; ORCiD logo [4]; ORCiD logo [8];  [4] more »;  [3] « less
  1. Univ. of Nebraska-Lincoln, NE (United States)
  2. Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford PULSE Inst.
  3. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  4. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford PULSE Inst.
  5. Univ. of Nebraska-Lincoln, Lincoln, NE (United States)
  6. Stanford Univ., CA (United States). Dept. of Physics
  7. Stony Brook Univ., NY (United States). Dept. of Physics and Astronomy
  8. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford PULSE Inst.; 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), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division; Melvin and Joan Lane Stanford Graduate Fellowship
OSTI Identifier:
1601104
Alternate Identifier(s):
OSTI ID: 1603722
Grant/Contract Number:  
[AC02-76SF00515; AC02-05-CH11231; SC0014170; AC0276SF00515]
Resource Type:
Accepted Manuscript
Journal Name:
Structural Dynamics
Additional Journal Information:
[ Journal Volume: 7; Journal Issue: 2]; Journal ID: ISSN 2329-7778
Publisher:
American Crystallographic Association/AIP
Country of Publication:
United States
Language:
English
Subject:
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS

Citation Formats

Nunes, J. P. F., Ledbetter, K., Lin, M., Kozina, M., DePonte, D. P., Biasin, E., Centurion, M., Crissman, C. J., Dunning, M., Guillet, S., Jobe, K., Liu, Y., Mo, M., Shen, X., Sublett, R., Weathersby, S., Yoneda, C., Wolf, Thomas J. A., Yang, J., Cordones, A. A., and Wang, X. J. Liquid-phase mega-electron-volt ultrafast electron diffraction. United States: N. p., 2020. Web. doi:10.1063/1.5144518.
Nunes, J. P. F., Ledbetter, K., Lin, M., Kozina, M., DePonte, D. P., Biasin, E., Centurion, M., Crissman, C. J., Dunning, M., Guillet, S., Jobe, K., Liu, Y., Mo, M., Shen, X., Sublett, R., Weathersby, S., Yoneda, C., Wolf, Thomas J. A., Yang, J., Cordones, A. A., & Wang, X. J. Liquid-phase mega-electron-volt ultrafast electron diffraction. United States. doi:10.1063/1.5144518.
Nunes, J. P. F., Ledbetter, K., Lin, M., Kozina, M., DePonte, D. P., Biasin, E., Centurion, M., Crissman, C. J., Dunning, M., Guillet, S., Jobe, K., Liu, Y., Mo, M., Shen, X., Sublett, R., Weathersby, S., Yoneda, C., Wolf, Thomas J. A., Yang, J., Cordones, A. A., and Wang, X. J. Mon . "Liquid-phase mega-electron-volt ultrafast electron diffraction". United States. doi:10.1063/1.5144518. https://www.osti.gov/servlets/purl/1601104.
@article{osti_1601104,
title = {Liquid-phase mega-electron-volt ultrafast electron diffraction},
author = {Nunes, J. P. F. and Ledbetter, K. and Lin, M. and Kozina, M. and DePonte, D. P. and Biasin, E. and Centurion, M. and Crissman, C. J. and Dunning, M. and Guillet, S. and Jobe, K. and Liu, Y. and Mo, M. and Shen, X. and Sublett, R. and Weathersby, S. and Yoneda, C. and Wolf, Thomas J. A. and Yang, J. and Cordones, A. A. and Wang, X. J.},
abstractNote = {The conversion of light into usable chemical and mechanical energy is pivotal to several biological and chemical processes, many of which occur in solution. To understand the structure–function relationships mediating these processes, a technique with high spatial and temporal resolutions is required. Here, we report on the design and commissioning of a liquid-phase mega-electron-volt (MeV) ultrafast electron diffraction instrument for the study of structural dynamics in solution. Limitations posed by the shallow penetration depth of electrons and the resulting information loss due to multiple scattering and the technical challenge of delivering liquids to vacuum were overcome through the use of MeV electrons and a gas-accelerated thin liquid sheet jet. To demonstrate the capabilities of this instrument, the structure of water and its network were resolved up to the 3rd hydration shell with a spatial resolution of 0.6 Å; preliminary time-resolved experiments demonstrated a temporal resolution of 200 fs.},
doi = {10.1063/1.5144518},
journal = {Structural Dynamics},
number = [2],
volume = [7],
place = {United States},
year = {2020},
month = {3}
}

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Works referenced in this record:

Liquid-Phase Electron Microscopy with Controllable Liquid Thickness
journal, June 2019


Heterogeneous to homogeneous melting transition visualized with ultrafast electron diffraction
journal, June 2018


Towards ETEM serial crystallography: Electron diffraction from liquid jets
journal, June 2011


Ultrafast Electron Diffraction and Structural Dynamics:  Transient Intermediates in the Elimination Reaction of C 2 F 4 I 2
journal, April 2002

  • Ihee, Hyotcherl; Goodson, Boyd M.; Srinivasan, Ramesh
  • The Journal of Physical Chemistry A, Vol. 106, Issue 16
  • DOI: 10.1021/jp014144r

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

The photochemical ring-opening of 1,3-cyclohexadiene imaged by ultrafast electron diffraction
journal, April 2019


Analysis of time-resolved X-ray scattering data from solution-state systems
journal, February 2010

  • Haldrup, Kristoffer; Christensen, Morten; Meedom Nielsen, Martin
  • Acta Crystallographica Section A Foundations of Crystallography, Vol. 66, Issue 2
  • DOI: 10.1107/S0108767309054233

On the calculation of x-ray scattering signals from pairwise radial distribution functions
journal, November 2015

  • Dohn, Asmus O.; Biasin, Elisa; Haldrup, Kristoffer
  • Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 48, Issue 24
  • DOI: 10.1088/0953-4075/48/24/244010

Ultrafast X-ray probing of water structure below the homogeneous ice nucleation temperature
journal, June 2014

  • Sellberg, J. A.; Huang, C.; McQueen, T. A.
  • Nature, Vol. 510, Issue 7505
  • DOI: 10.1038/nature13266

Femtosecond gas phase electron diffraction with MeV electrons
journal, January 2016

  • Yang, Jie; Guehr, Markus; Vecchione, Theodore
  • Faraday Discussions, Vol. 194
  • DOI: 10.1039/C6FD00071A

Molecular dynamics with coupling to an external bath
journal, October 1984

  • Berendsen, H. J. C.; Postma, J. P. M.; van Gunsteren, W. F.
  • The Journal of Chemical Physics, Vol. 81, Issue 8
  • DOI: 10.1063/1.448118

More accurate X-ray scattering data of deeply supercooled bulk liquid water
journal, January 2011


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

GROMACS: Fast, flexible, and free
journal, January 2005

  • Van Der Spoel, David; Lindahl, Erik; Hess, Berk
  • Journal of Computational Chemistry, Vol. 26, Issue 16
  • DOI: 10.1002/jcc.20291

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

Bond Dissociation Triggering Molecular Disorder in Amorphous H 2 O
journal, November 2018

  • Hada, Masaki; Shigeeda, Yuho; Koshihara, Shin-ya
  • The Journal of Physical Chemistry A, Vol. 122, Issue 49
  • DOI: 10.1021/acs.jpca.8b08455

Anomalous Behavior of the Homogeneous Ice Nucleation Rate in “No-Man’s Land”
journal, July 2015

  • Laksmono, Hartawan; McQueen, Trevor A.; Sellberg, Jonas A.
  • The Journal of Physical Chemistry Letters, Vol. 6, Issue 14
  • DOI: 10.1021/acs.jpclett.5b01164

High flow rate nanofluidics for in-liquid electron microscopy and diffraction
journal, July 2019


Electron inelastic mean free path formula and CSDA-range calculation in biological compounds for low and intermediate energies
journal, May 2006


Development of an improved four-site water model for biomolecular simulations: TIP4P-Ew
journal, May 2004

  • Horn, Hans W.; Swope, William C.; Pitera, Jed W.
  • The Journal of Chemical Physics, Vol. 120, Issue 20
  • DOI: 10.1063/1.1683075

Dynamics of Light Harvesting in Photosynthesis
journal, May 2009


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

Nanofluidic Cells with Controlled Pathlength and Liquid Flow for Rapid, High-Resolution In Situ Imaging with Electrons
journal, June 2013

  • Mueller, C.; Harb, M.; Dwyer, J. R.
  • The Journal of Physical Chemistry Letters, Vol. 4, Issue 14
  • DOI: 10.1021/jz401067k

A direct electron detector for time-resolved MeV electron microscopy
journal, March 2017

  • Vecchione, T.; Denes, P.; Jobe, R. K.
  • Review of Scientific Instruments, Vol. 88, Issue 3
  • DOI: 10.1063/1.4977923

Ultrafast Electron Crystallography of Interfacial Water
journal, April 2004


Parametric study on impinging-jet liquid sheet thickness distribution using an interferometric method
journal, July 2001


Device design and flow scaling for liquid sheet jets
journal, November 2018


Generation and characterization of ultrathin free-flowing liquid sheets
journal, April 2018


Benchmark oxygen-oxygen pair-distribution function of ambient water from x-ray diffraction measurements with a wide Q -range
journal, February 2013

  • Skinner, Lawrie B.; Huang, Congcong; Schlesinger, Daniel
  • The Journal of Chemical Physics, Vol. 138, Issue 7
  • DOI: 10.1063/1.4790861

Diffraction and IR/Raman data do not prove tetrahedral water
journal, August 2008

  • Leetmaa, Mikael; Wikfeldt, Kjartan Thor; Ljungberg, Mathias P.
  • The Journal of Chemical Physics, Vol. 129, Issue 8
  • DOI: 10.1063/1.2968550

Thymine Dimerization in DNA Is an Ultrafast Photoreaction
journal, February 2007


Investigation of amorphous materials by electron diffraction — The effects of multiple scattering
journal, January 1988


Ultrafast X-ray Diffraction of Transient Molecular Structures in Solution
journal, August 2005


VMD: Visual molecular dynamics
journal, February 1996


Electron diffraction on liquid water
journal, March 1974

  • Lengyel, SÁNdor; KÁLmÁN, Erika
  • Nature, Vol. 248, Issue 5447
  • DOI: 10.1038/248405a0

Diffractive imaging of dissociation and ground-state dynamics in a complex molecule
journal, August 2019


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

A molecular beam study of the evaporation of water from a liquid jet
journal, June 1988

  • Faubel, M.; Schlemmer, S.; Toennies, J. P.
  • Zeitschrift f�r Physik D Atoms, Molecules and Clusters, Vol. 10, Issue 2-3
  • DOI: 10.1007/BF01384861

Conical intersection dynamics of the primary photoisomerization event in vision
journal, September 2010

  • Polli, Dario; Altoè, Piero; Weingart, Oliver
  • Nature, Vol. 467, Issue 7314
  • DOI: 10.1038/nature09346

X-ray and Neutron Scattering of Water
journal, April 2016

  • Amann-Winkel, Katrin; Bellissent-Funel, Marie-Claire; Bove, Livia E.
  • Chemical Reviews, Vol. 116, Issue 13
  • DOI: 10.1021/acs.chemrev.5b00663