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Updated: May 3, 2026

Author Spotlight: Unveiling the Potential of VSFG Microscopy in Studying Mesoscopically Heterogeneous Self-Assembled Structures
Published on: December 1, 2023
Axis-dependence of molecular high harmonic emission in three dimensions
Limor S Spector1, Maxim Artamonov2, Shungo Miyabe3
11] Applied Physics Department, 382 Via Pueblo Mall, Stanford University, Stanford, California 94305, USA [2] Stanford PULSE Institute, 2575 Sand Hill Road, SLAC National Accelerator Laboratory, Menlo Park, California 94025, USA.
Abstract:
High-order harmonic generation in an atomic or molecular gas is a promising source of sub-femtosecond vacuum ultraviolet coherent radiation for transient scattering, absorption, metrology and imaging applications. High harmonic spectra are sensitive to Ångstrom-scale structure and motion of laser-driven molecules, but interference from radiation produced by random molecular orientations obscures this in all but the simplest cases, such as linear molecules. Here we show how to extract full body-frame high harmonic generation information for molecules with more complicated geometries by utilizing the methods of coherent transient rotational spectroscopy. To demonstrate this approach, we obtain the relative strength of harmonic emission along the three principal axes in the asymmetric-top sulphur dioxide. This greatly simplifies the analysis task of high harmonic spectroscopy and extends its usefulness to more complex molecules.
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