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Picosecond pulse-shaping for strong three-dimensional field-free alignment of generic asymmetric-top molecules

Author

Listed:
  • Terry Mullins

    (Deutsches Elektronen-Synchrotron DESY)

  • Evangelos T. Karamatskos

    (Deutsches Elektronen-Synchrotron DESY
    Universität Hamburg)

  • Joss Wiese

    (Deutsches Elektronen-Synchrotron DESY
    Universität Hamburg
    Universität of Hamburg)

  • Jolijn Onvlee

    (Deutsches Elektronen-Synchrotron DESY
    Universität of Hamburg
    Radboud University)

  • Arnaud Rouzée

    (Max Born Institute)

  • Andrey Yachmenev

    (Deutsches Elektronen-Synchrotron DESY
    Universität of Hamburg)

  • Sebastian Trippel

    (Deutsches Elektronen-Synchrotron DESY
    Universität of Hamburg)

  • Jochen Küpper

    (Deutsches Elektronen-Synchrotron DESY
    Universität Hamburg
    Universität Hamburg
    Universität of Hamburg)

Abstract

Fixing molecules in space is a crucial step for the imaging of molecular structure and dynamics. Here, we demonstrate three-dimensional (3D) field-free alignment of the prototypical asymmetric top molecule indole using elliptically polarized, shaped, off-resonant laser pulses. A truncated laser pulse is produced using a combination of extreme linear chirping and controlled phase and amplitude shaping using a spatial-light-modulator (SLM) based pulse shaper of a broadband laser pulse. The angular confinement is detected through velocity-map imaging of H+ and C2+ fragments resulting from strong-field ionization and Coulomb explosion of the aligned molecules by intense femtosecond laser pulses. The achieved three-dimensional alignment is characterized by comparing the result of ion-velocity-map measurements for different alignment directions and for different times during and after the alignment laser pulse to accurate computational results. The achieved strong three-dimensional field-free alignment of $$ =0.89$$ = 0.89 demonstrates the feasibility of both, strong three-dimensional alignment of generic complex molecules and its quantitative characterization.

Suggested Citation

  • Terry Mullins & Evangelos T. Karamatskos & Joss Wiese & Jolijn Onvlee & Arnaud Rouzée & Andrey Yachmenev & Sebastian Trippel & Jochen Küpper, 2022. "Picosecond pulse-shaping for strong three-dimensional field-free alignment of generic asymmetric-top molecules," Nature Communications, Nature, vol. 13(1), pages 1-7, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-28951-z
    DOI: 10.1038/s41467-022-28951-z
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    References listed on IDEAS

    as
    1. Evangelos T. Karamatskos & Sebastian Raabe & Terry Mullins & Andrea Trabattoni & Philipp Stammer & Gildas Goldsztejn & Rasmus R. Johansen & Karol Długołecki & Henrik Stapelfeldt & Marc J. J. Vrakking , 2019. "Molecular movie of ultrafast coherent rotational dynamics of OCS," Nature Communications, Nature, vol. 10(1), pages 1-7, December.
    2. Jie Yang & Markus Guehr & Theodore Vecchione & Matthew S. Robinson & Renkai Li & Nick Hartmann & Xiaozhe Shen & Ryan Coffee & Jeff Corbett & Alan Fry & Kelly Gaffney & Tais Gorkhover & Carsten Hast & , 2016. "Diffractive imaging of a rotational wavepacket in nitrogen molecules with femtosecond megaelectronvolt electron pulses," Nature Communications, Nature, vol. 7(1), pages 1-9, September.
    3. Hiromichi Niikura & F. Légaré & R. Hasbani & A. D. Bandrauk & Misha Yu. Ivanov & D. M. Villeneuve & P. B. Corkum, 2002. "Sub-laser-cycle electron pulses for probing molecular dynamics," Nature, Nature, vol. 417(6892), pages 917-922, June.
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    5. Samuel G. Walt & Niraghatam Bhargava Ram & Marcos Atala & Nikolay I Shvetsov-Shilovski & Aaron von Conta & Denitsa Baykusheva & Manfred Lein & Hans Jakob Wörner, 2017. "Dynamics of valence-shell electrons and nuclei probed by strong-field holography and rescattering," Nature Communications, Nature, vol. 8(1), pages 1-8, August.
    6. Andrea Trabattoni & Joss Wiese & Umberto Giovannini & Jean-François Olivieri & Terry Mullins & Jolijn Onvlee & Sang-Kil Son & Biagio Frusteri & Angel Rubio & Sebastian Trippel & Jochen Küpper, 2020. "Setting the photoelectron clock through molecular alignment," Nature Communications, Nature, vol. 11(1), pages 1-7, December.
    7. J. Itatani & J. Levesque & D. Zeidler & Hiromichi Niikura & H. Pépin & J. C. Kieffer & P. B. Corkum & D. M. Villeneuve, 2004. "Tomographic imaging of molecular orbitals," Nature, Nature, vol. 432(7019), pages 867-871, December.
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