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Updated: Feb 17, 2026

Direct Imaging of Laser-driven Ultrafast Molecular Rotation
Published on: February 4, 2017
Laser-induced blurring of molecular structure information in high harmonic spectroscopy
François Risoud1, Camille Lévêque1,2,3, Marie Labeye1
1Sorbonne Université, UPMC Univ. Paris 6, CNRS-UMR 7614, Laboratoire de Chimie Physique-Matière et Rayonnement, 4 place Jussieu, 75252, Paris Cedex 05, France.
Abstract:
High harmonic spectroscopy gives access to molecular structure with Angström resolution. Such information is encoded in the destructive interferences occurring between the harmonic emissions from the different parts of the molecule. By solving the time-dependent Schrödinger equation, either numerically or with the molecular strong-field approximation, we show that the electron dynamics in the emission process generally results in a strong spectral smoothing of the interferences, blurring the structural information. However we identify specific generation conditions where they are unaffected. These findings have important consequences for molecular imaging and orbital tomography using high harmonic spectroscopy.
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