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.

8 pages, 6 figures

References in corpus (7)

• Quantitative Rescattering Theory for high-order harmonic generation from molecules
• Attosecond probing of nuclear dynamics with trajectory-resolved high-harmonic spectroscopy
• Photoelectron holographic interferometry to probe the longitudinal momentum offset at the tunnel exit
• Uncovering multiple orbitals influence in high harmonic generation from aligned N${}_2$
• Visualizing molecular unidirectional rotation
• H2 Double Ionization with Few-Cycle Laser Pulses
• Orientation Resolution through Rotational Coherence Spectroscopy

Cited by in corpus (3)

• 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
• Imaging the geometrical structure of complex symmetric molecules by above-threshold ionization spectrum in an IR+XUV laser field