Journal
NATURE COMMUNICATIONS
Volume 13, Issue 1, Pages -Publisher
NATURE PORTFOLIO
DOI: 10.1038/s41467-022-28951-z
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Funding
- Deutsche Forschungsgemeinschaft (DFG) through the priority program Quantum Dynamics in Tailored Intense Fields (QUTIF) [SPP1840, KU 1527/3, AR 4577/4, YA 610/1]
- Cluster of Excellence Center for Ultrafast Imaging (CUI, EXC 1074) [194651731]
- Cluster of Excellence Advanced Imaging of Matter (AIM, EXC 2056) [390715994]
- European Research Council under the European Union's Seventh Framework Programme (FP7/2007-2013) through the Consolidator Grant COMOTION [614507]
- Alexander von Humboldt Foundation
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This study demonstrates a method for achieving three-dimensional field-free alignment using off-resonant laser pulses, and verifies its applicability and quantitative characteristics for complex molecules through experiments.
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 demonstrates the feasibility of both, strong three-dimensional alignment of generic complex molecules and its quantitative characterization.
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