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

2020/09/17 by Terry Mullins, Evangelos Karamatskos, Mullins, Terry +13 · 1 citation
Physics and Astronomy · #Advanced Fiber Laser Technologies #Atomic and Molecular Clusters (physics.atm-clus) #Chemical Physics (physics.chem-ph) #FOS: Physical sciences #Laser-Matter Interactions and Applications #Laser-Plasma Interactions and Diagnostics

paper · pdf · doi:10.48550/arxiv.2009.08157

openalex publication_date 2020/09/17 · openalex created_date 2022/07/25 · openalex updated_date 2026/07/28

Abstract

Fixing molecules in space is a crucial step for the imaging of molecular\nstructure and dynamics. Here, we demonstrate three-dimensional (3D) field-free\nalignment of the prototypical asymmetric top molecule indole using elliptically\npolarized, shaped, off-resonant laser pulses. A truncated laser pulse is\nproduced using a combination of extreme linear chirping and controlled phase\nand amplitude shaping using a spatial-light-modulator (SLM) based pulse shaper\nof a broadband laser pulse. The angular confinement is detected through\nvelocity-map imaging of H+ and C2+ fragments resulting from\nstrong-field ionization and Coulomb explosion of the aligned molecules by\nintense femtosecond laser pulses. The achieved three-dimensional alignment is\ncharacterized by comparing the result of ion-velocity-map measurements for\ndifferent alignment directions and for different times during and after the\nalignment laser pulse to accurate computational results. The achieved strong\nthree-dimensional field-free alignment of \⟨ \cos2\δ \⟩=0.89\ndemonstrates the feasibility of both, strong three-dimensional alignment of\ngeneric complex molecules and its quantitative characterization.\n

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