Molecular rotation movie filmed with high-harmonic generation

Abstract

Direct imaging of molecular dynamics is a long-standing goal in physics and chemistry. As an emerging tool, high-harmonic spectroscopy (HHS) enables accessing molecular dynamics on femtosecond to attosecond time scales. However, decoding information from the harmonic signals is usually painstaking due to the coherent nature of high-harmonic generation (HHG). Here we show that this obstacle can be effectively overcome by exploiting machine learning in HHS. Combining the machine learning with an angle-resolved HHS method, we demonstrate that the rich dynamics of molecular rotational wave packet is fully reconstructed from the angular distributions of HHG measured at various time delays of the probe pulse. The experimental retrievals are in good agreement with the numerical simulations. These findings provide a comprehensive picture of molecular rotation in space and time which will facilitate the development of related researches on molecular dynamics imaging.

arXiv comment8 pages, 6 figures

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Cited by in corpus (6)

• All-optical measurement of high-order fractional molecular echoes by high-order harmonic generation
• Exit momentum and instantaneous ionization rate of nonadiabatic tunneling ionization in elliptically polarized laser fields
• Optical imaging of coherent molecular rotors
• Rotation of polarization of light propagating through a gas of molecular super-rotors
• Visualizing coherent molecular rotation in a gaseous medium
• Imaging the geometrical structure of complex symmetric molecules by above-threshold ionization spectrum in an IR+XUV laser field