Journal Article PUBDB-2022-01584

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

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2022
Nature Publishing Group UK [London]

Nature Communications 13(1), 1431 () [10.1038/s41467-022-28951-z]
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Report No.: arXiv:2009.08157

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 proto- typical 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 C$^{2+}$ 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 <$cos^{2}δ4$> 0:89 demonstrates the feasibility of both, strong three-dimensional alignment of generic complex molecules and its quantitative characterization.

Classification:

Contributing Institute(s):
  1. CFEL-CMI (FS-CFEL-CMI)
  2. beauftragt von UNI (UNI/CUI)
  3. Uni Hamburg / Experimentalphysik (UNI/EXP)
Research Program(s):
  1. 631 - Matter – Dynamics, Mechanisms and Control (POF4-631) (POF4-631)
  2. MEDEA - Molecular Electron Dynamics investigated by IntensE Fields and Attosecond Pulses (641789) (641789)
  3. DFG project 390715994 - EXC 2056: CUI: Advanced Imaging of Matter (390715994) (390715994)
  4. COMOTION - Controlling the Motion of Complex Molecules and Particles (614507) (614507)
  5. DFG project 194651731 - EXC 1074: Hamburger Zentrum für ultraschnelle Beobachtung (CUI): Struktur, Dynamik und Kontrolle von Materie auf atomarer Skala (194651731) (194651731)
Experiment(s):
  1. Experiments at CFEL

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Picosecond pulse-shaping for strong three-dimensional field-free alignment of generic asymmetric-top molecules
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 Record created 2022-03-22, last modified 2025-07-15