Visualizing complex-amplitude assembly in high-order harmonic generation from oriented polar molecules
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Updated: Nov 1, 2026

Direct Imaging of Laser-driven Ultrafast Molecular Rotation
Published on: February 4, 2017
Tianqi Ruan1, Chaojin Zhang1, Lihao Weng1
1School of Physics and Optoelectronic Engineering, Jiangsu Normal University, Xuzhou 221116, China.
Abstract:
Polarization-resolved high-order harmonic generation from oriented polar molecules encodes electron recollision from opposite molecular directions, yet the underlying interference is hidden in intensity spectra. Here we decompose the polarization-resolved harmonic response of carbon monoxide molecules into four ionization-recombination amplitudes associated with the carbon and oxygen centers. The calculated spectra reproduce the established odd-even polarization pattern and reveal distinct orientation-dependent behavior for neighboring harmonics near the cutoff. Molecular rotation converts destructive interference into phase locking of the carbon-ionization amplitudes for the even harmonic, whereas increasing phase competition suppresses the neighboring odd harmonic. This contrast is manifested in the orientation-dependent polarized yields, the polarization imbalance, and the contrasting activation and suppression of neighboring harmonics, providing experimentally accessible signatures of microscopic interference in oriented polar molecules.
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