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Title: Strongly aligned gas-phase molecules at free-electron lasers

Abstract

Here, we demonstrate a novel experimental implementation to strongly align molecules at full repetition rates of free-electron lasers. We utilized the available in-house laser system at the coherent x-ray imaging beamline at the linac coherent light source. Chirped laser pulses, i.e., the direct output from the regenerative amplifier of the Ti:Sa chirped pulse amplification laser system, were used to strongly align 2, 5-diiodothiophene molecules in a molecular beam. The alignment laser pulses had pulse energies of a few mJ and a pulse duration of 94 ps. A degree of alignment of $$\langle {\mathrm{cos}}^{2}{\theta }_{2{\rm{D}}}\rangle =0.85$$ was measured, limited by the intrinsic temperature of the molecular beam rather than by the available laser system. With the general availability of synchronized chirped-pulse-amplified near-infrared laser systems at short-wavelength laser facilities, our approach allows for the universal preparation of molecules tightly fixed in space for experiments with x-ray pulses.

Authors:
 [1];  [2];  [2];  [3];  [3];  [2];  [4];  [2];  [3];  [5];  [1];  [6];  [7];  [3];  [3];  [3];  [2];  [2];  [8];  [8] more »;  [9];  [10];  [11];  [6];  [2];  [6];  [12];  [13];  [2];  [1] « less
  1. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); Univ. of Hamburg, Hamburg (Germany)
  2. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)
  3. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  4. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); European X-ray Free Electron Laser (XFEL), GmbH, Hamburg (Germany)
  5. SLAC National Accelerator Lab., Menlo Park, CA (United States); PULSE Institute, Stanford, CA (United States). SLAC National Accelerator Lab.; Stanford Univ., Stanford, CA (United States)
  6. Aarhus Univ., Aarhus (Denmark)
  7. SLAC National Accelerator Lab., Menlo Park, CA (United States); PULSE Institute, Stanford, CA (United States). SLAC National Accelerator Lab.
  8. PULSE Institute, Stanford, CA (United States). SLAC National Accelerator Lab.
  9. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); Kansas State Univ., Manhattan, KS (United States)
  10. Kansas State Univ., Manhattan, KS (United States)
  11. Max Planck Institute for Nuclear Physics, Heidelberg (Germany)
  12. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); European X-ray Free Electron Laser (XFEL) GmbH, Hamburg (Germany)
  13. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); 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:
1263392
Alternate Identifier(s):
OSTI ID: 1238841
Report Number(s):
SLAC-PUB-16644
Journal ID: ISSN 0953-4075; arXiv:1506.03650
Grant/Contract Number:  
AC02-76SF00515
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physics. B, Atomic, Molecular and Optical Physics
Additional Journal Information:
Journal Volume: 48; Journal Issue: 20; Journal ID: ISSN 0953-4075
Publisher:
IOP Publishing
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS; PHYS; molecular physics; controlled molecules; alignment; free-electron laser; imaging; coherent diffractive imaging; laser control

Citation Formats

Kierspel, Thomas, Wiese, Joss, Mullins, Terry, Robinson, Joseph, Aquila, Andy, Barty, Anton, Bean, Richard, Boll, Rebecca, Boutet, Sebastien, Bucksbaum, Philip, Chapman, Henry N., Christensen, Lauge, Fry, Alan, Hunter, Mark, Koglin, Jason E., Liang, Mengning, Mariani, Valerio, Morgan, Andrew, Natan, Adi, Petrovic, Vladimir, Rolles, Daniel, Rudenko, Artem, Schnorr, Kirsten, Stapelfeldt, Henrik, Stern, Stephan, Thogersen, Jan, Yoon, Chun Hong, Wang, Fenglin, Trippel, Sebastian, and Kupper, Jochen. Strongly aligned gas-phase molecules at free-electron lasers. United States: N. p., 2015. Web. doi:10.1088/0953-4075/48/20/204002.
Kierspel, Thomas, Wiese, Joss, Mullins, Terry, Robinson, Joseph, Aquila, Andy, Barty, Anton, Bean, Richard, Boll, Rebecca, Boutet, Sebastien, Bucksbaum, Philip, Chapman, Henry N., Christensen, Lauge, Fry, Alan, Hunter, Mark, Koglin, Jason E., Liang, Mengning, Mariani, Valerio, Morgan, Andrew, Natan, Adi, Petrovic, Vladimir, Rolles, Daniel, Rudenko, Artem, Schnorr, Kirsten, Stapelfeldt, Henrik, Stern, Stephan, Thogersen, Jan, Yoon, Chun Hong, Wang, Fenglin, Trippel, Sebastian, & Kupper, Jochen. Strongly aligned gas-phase molecules at free-electron lasers. United States. doi:10.1088/0953-4075/48/20/204002.
Kierspel, Thomas, Wiese, Joss, Mullins, Terry, Robinson, Joseph, Aquila, Andy, Barty, Anton, Bean, Richard, Boll, Rebecca, Boutet, Sebastien, Bucksbaum, Philip, Chapman, Henry N., Christensen, Lauge, Fry, Alan, Hunter, Mark, Koglin, Jason E., Liang, Mengning, Mariani, Valerio, Morgan, Andrew, Natan, Adi, Petrovic, Vladimir, Rolles, Daniel, Rudenko, Artem, Schnorr, Kirsten, Stapelfeldt, Henrik, Stern, Stephan, Thogersen, Jan, Yoon, Chun Hong, Wang, Fenglin, Trippel, Sebastian, and Kupper, Jochen. Wed . "Strongly aligned gas-phase molecules at free-electron lasers". United States. doi:10.1088/0953-4075/48/20/204002. https://www.osti.gov/servlets/purl/1263392.
@article{osti_1263392,
title = {Strongly aligned gas-phase molecules at free-electron lasers},
author = {Kierspel, Thomas and Wiese, Joss and Mullins, Terry and Robinson, Joseph and Aquila, Andy and Barty, Anton and Bean, Richard and Boll, Rebecca and Boutet, Sebastien and Bucksbaum, Philip and Chapman, Henry N. and Christensen, Lauge and Fry, Alan and Hunter, Mark and Koglin, Jason E. and Liang, Mengning and Mariani, Valerio and Morgan, Andrew and Natan, Adi and Petrovic, Vladimir and Rolles, Daniel and Rudenko, Artem and Schnorr, Kirsten and Stapelfeldt, Henrik and Stern, Stephan and Thogersen, Jan and Yoon, Chun Hong and Wang, Fenglin and Trippel, Sebastian and Kupper, Jochen},
abstractNote = {Here, we demonstrate a novel experimental implementation to strongly align molecules at full repetition rates of free-electron lasers. We utilized the available in-house laser system at the coherent x-ray imaging beamline at the linac coherent light source. Chirped laser pulses, i.e., the direct output from the regenerative amplifier of the Ti:Sa chirped pulse amplification laser system, were used to strongly align 2, 5-diiodothiophene molecules in a molecular beam. The alignment laser pulses had pulse energies of a few mJ and a pulse duration of 94 ps. A degree of alignment of $\langle {\mathrm{cos}}^{2}{\theta }_{2{\rm{D}}}\rangle =0.85$ was measured, limited by the intrinsic temperature of the molecular beam rather than by the available laser system. With the general availability of synchronized chirped-pulse-amplified near-infrared laser systems at short-wavelength laser facilities, our approach allows for the universal preparation of molecules tightly fixed in space for experiments with x-ray pulses.},
doi = {10.1088/0953-4075/48/20/204002},
journal = {Journal of Physics. B, Atomic, Molecular and Optical Physics},
number = 20,
volume = 48,
place = {United States},
year = {2015},
month = {9}
}

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Works referenced in this record:

Laser-Induced Electron Tunneling and Diffraction
journal, June 2008


Photoelectron angular distributions from strong-field ionization of oriented molecules
journal, May 2010

  • Holmegaard, Lotte; Hansen, Jonas L.; Kalhøj, Line
  • Nature Physics, Vol. 6, Issue 6
  • DOI: 10.1038/nphys1666

Femtosecond photoelectron diffraction on laser-aligned molecules: Towards time-resolved imaging of molecular structure
journal, December 2013


Tomographic imaging of molecular orbitals
journal, December 2004


Following a chemical reaction using high-harmonic interferometry
journal, July 2010

  • Wörner, H. J.; Bertrand, J. B.; Kartashov, D. V.
  • Nature, Vol. 466, Issue 7306
  • DOI: 10.1038/nature09185

Laser-induced electron diffraction: a new tool for probing ultrafast molecular dynamics
journal, September 1996


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 of Isolated Molecules with Ultrafast Electron Pulses
journal, September 2012


Femtosecond electron diffraction: heralding the era of atomically resolved dynamics
journal, August 2011


X-Ray Diffraction from Isolated and Strongly Aligned Gas-Phase Molecules with a Free-Electron Laser
journal, February 2014


Molecular Imaging Using X-Ray Free-Electron Lasers
journal, April 2013


Colloquium : Aligning molecules with strong laser pulses
journal, April 2003


State- and conformer-selected beams of aligned and oriented molecules for ultrafast diffraction studies
journal, January 2011

  • Filsinger, Frank; Meijer, Gerard; Stapelfeldt, Henrik
  • Phys. Chem. Chem. Phys., Vol. 13, Issue 6
  • DOI: 10.1039/C0CP01585G

Spectroscopy of pendular states: The use of molecular complexes in achieving orientation
journal, March 1992


Laser-induced molecular alignment probed by a double-pulse experiment
journal, October 1992

  • Normand, D.; Lompre, L. A.; Cornaggia, C.
  • Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 25, Issue 20
  • DOI: 10.1088/0953-4075/25/20/001

Experimental Observation of Revival Structures in Picosecond Laser-Induced Alignment of I2
journal, September 2001


Controlling the alignment of neutral molecules by a strong laser field
journal, June 1999

  • Sakai, Hirofumi; Safvan, C. P.; Larsen, Jakob Juul
  • The Journal of Chemical Physics, Vol. 110, Issue 21
  • DOI: 10.1063/1.478039

Laser-Induced Alignment and Orientation of Quantum-State-Selected Large Molecules
journal, January 2009


Impulsive orientation and alignment of quantum-state-selected NO molecules
journal, March 2009

  • Ghafur, Omair; Rouzée, Arnaud; Gijsbertsen, Arjan
  • Nature Physics, Vol. 5, Issue 4
  • DOI: 10.1038/nphys1225

Quantum-state selection, alignment, and orientation of large molecules using static electric and laser fields
journal, January 2009

  • Filsinger, Frank; Küpper, Jochen; Meijer, Gerard
  • The Journal of Chemical Physics, Vol. 131, Issue 6
  • DOI: 10.1063/1.3194287

Three Dimensional Alignment of Molecules Using Elliptically Polarized Laser Fields
journal, September 2000


Field-Free Three-Dimensional Alignment of Polyatomic Molecules
journal, October 2006


Multipulse Three-Dimensional Alignment of Asymmetric Top Molecules
journal, April 2014


Three-dimensional molecular orientation with combined electrostatic and elliptically polarized laser fields
journal, December 2005


Computational studies of x-ray scattering from three-dimensionally-aligned asymmetric-top molecules
journal, April 2010


Role of rotational temperature in adiabatic molecular alignment
journal, November 2006

  • Kumarappan, Vinod; Bisgaard, Christer Z.; Viftrup, Simon S.
  • The Journal of Chemical Physics, Vol. 125, Issue 19
  • DOI: 10.1063/1.2388273

Time evolution of pendular states created by the interaction of molecular polarizability with a pulsed nonresonant laser field
journal, February 1999

  • Ortigoso, Juan; Rodrı́guez, Mirta; Gupta, Manish
  • The Journal of Chemical Physics, Vol. 110, Issue 8
  • DOI: 10.1063/1.478241

Dynamics of laser-induced molecular alignment in the impulsive and adiabatic regimes: A direct comparison
journal, August 2005


Laser-induced alignment and anti-alignment of rotationally excited molecules
journal, January 2011

  • Owschimikow, Nina; Schmidt, Burkhard; Schwentner, Nikolaus
  • Physical Chemistry Chemical Physics, Vol. 13, Issue 19
  • DOI: 10.1039/c0cp02260h

Strongly aligned and oriented molecular samples at a kHz repetition rate
journal, June 2013


Strongly driven quantum pendulum of the carbonyl sulfide molecule
journal, May 2014


The Coherent X-ray Imaging (CXI) instrument at the Linac Coherent Light Source (LCLS)
journal, March 2010


The Coherent X-ray Imaging instrument at the Linac Coherent Light Source
journal, April 2015

  • Liang, Mengning; Williams, Garth J.; Messerschmidt, Marc
  • Journal of Synchrotron Radiation, Vol. 22, Issue 3
  • DOI: 10.1107/S160057751500449X

Field-free molecular alignment probed by the free electron laser in Hamburg (FLASH)
journal, June 2009

  • Johnsson, P.; Rouzée, A.; Siu, W.
  • Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 42, Issue 13
  • DOI: 10.1088/0953-4075/42/13/134017

Time-resolved pump-probe experiments at the LCLS
journal, January 2010

  • Glownia, James M.; Cryan, J.; Andreasson, J.
  • Optics Express, Vol. 18, Issue 17
  • DOI: 10.1364/OE.18.017620

Auger Electron Angular Distribution of Double Core-Hole States in the Molecular Reference Frame
journal, August 2010


Femtosecond x-ray photoelectron diffraction on gas-phase dibromobenzene molecules
journal, June 2014


Imaging molecular structure through femtosecond photoelectron diffraction on aligned and oriented gas-phase molecules
journal, January 2014

  • Boll, Rebecca; Rouzée, Arnaud; Adolph, Marcus
  • Faraday Discuss., Vol. 171
  • DOI: 10.1039/C4FD00037D

Toward atomic resolution diffractive imaging of isolated molecules with X-ray free-electron lasers
journal, January 2014

  • Stern, S.; Holmegaard, L.; Filsinger, F.
  • Faraday Discuss., Vol. 171
  • DOI: 10.1039/C4FD00028E

Cooling of large molecules below 1 K and He clusters formation
journal, May 2000

  • Even, U.; Jortner, J.; Noy, D.
  • The Journal of Chemical Physics, Vol. 112, Issue 18
  • DOI: 10.1063/1.481405

Cheetah : software for high-throughput reduction and analysis of serial femtosecond X-ray diffraction data
journal, May 2014

  • Barty, Anton; Kirian, Richard A.; Maia, Filipe R. N. C.
  • Journal of Applied Crystallography, Vol. 47, Issue 3
  • DOI: 10.1107/S1600576714007626

A system for Coulomb explosion imaging of small molecules at the Weizmann Institute
journal, June 1993

  • Kella, D.; Algranati, M.; Feldman, H.
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 329, Issue 3
  • DOI: 10.1016/0168-9002(93)91279-V

Improved two-dimensional product imaging: The real-time ion-counting method
journal, April 1998

  • Chang, Bor-Yu; Hoetzlein, Rama C.; Mueller, Julie A.
  • Review of Scientific Instruments, Vol. 69, Issue 4
  • DOI: 10.1063/1.1148824

Time‐of‐Flight Mass Spectrometer with Improved Resolution
journal, December 1955

  • Wiley, W. C.; McLaren, I. H.
  • Review of Scientific Instruments, Vol. 26, Issue 12
  • DOI: 10.1063/1.1715212

Velocity map imaging of ions and electrons using electrostatic lenses: Application in photoelectron and photofragment ion imaging of molecular oxygen
journal, September 1997

  • Eppink, André T. J. B.; Parker, David H.
  • Review of Scientific Instruments, Vol. 68, Issue 9
  • DOI: 10.1063/1.1148310

Aligning molecules with intense nonresonant laser fields
journal, November 1999

  • Larsen, Jakob Juul; Sakai, Hirofumi; Safvan, C. P.
  • The Journal of Chemical Physics, Vol. 111, Issue 17
  • DOI: 10.1063/1.480112

Mixed-field orientation of molecules without rotational symmetry
journal, December 2013

  • Hansen, Jonas L.; Omiste, Juan J.; Nielsen, Jens H.
  • The Journal of Chemical Physics, Vol. 139, Issue 23
  • DOI: 10.1063/1.4848735

Generation and Propagation of Intense Supersonic Beams
journal, June 2011

  • Luria, K.; Christen, W.; Even, U.
  • The Journal of Physical Chemistry A, Vol. 115, Issue 25
  • DOI: 10.1021/jp201342u

Diffraction and imaging from a beam of laser-aligned proteins: resolution limits
journal, February 2005

  • Spence, J. C. H.; Schmidt, K.; Wu, J. S.
  • Acta Crystallographica Section A Foundations of Crystallography, Vol. 61, Issue 2
  • DOI: 10.1107/S0108767305002710

Recoil-ion and electron momentum spectroscopy: reaction-microscopes
journal, August 2003


Strongly aligned and oriented molecular samples at a kHz repetition rate
text, January 2013

  • Trippel, Sebastian; Mullins, Terence; Müller, Nele Lotte Marie
  • Deutsches Elektronen-Synchrotron, DESY, Hamburg
  • DOI: 10.3204/desy-2014-02100

    Works referencing / citing this record:

    Räumliche Trennung der Konformere eines Dipeptids
    journal, September 2018

    • Teschmit, Nicole; Horke, Daniel A.; Küpper, Jochen
    • Angewandte Chemie, Vol. 130, Issue 42
    • DOI: 10.1002/ange.201807646

    Spatially Separating the Conformers of a Dipeptide
    journal, October 2018

    • Teschmit, Nicole; Horke, Daniel A.; Küpper, Jochen
    • Angewandte Chemie International Edition, Vol. 57, Issue 42
    • DOI: 10.1002/anie.201807646

    OnDA : online data analysis and feedback for serial X-ray imaging
    journal, May 2016

    • Mariani, Valerio; Morgan, Andrew; Yoon, Chun Hong
    • Journal of Applied Crystallography, Vol. 49, Issue 3
    • DOI: 10.1107/s1600576716007469

    The LAMP instrument at the Linac Coherent Light Source free-electron laser
    text, January 2018

    • Osipov, Timur; Bostedt, Christoph; Castagna, J. -C.
    • Deutsches Elektronen-Synchrotron, DESY, Hamburg
    • DOI: 10.3204/pubdb-2019-00069