High-harmonic generation from arbitrarily oriented diatomic molecules including nuclear motion and field-free alignment

Abstract

We present a theoretical model of high-harmonic generation from diatomic molecules. The theory includes effects of alignment as well as nuclear motion and is used to predict results for N${}_2$, O${}_2$, H${}_2$ and D${}_2$. The results show that the alignment dependence of high-harmonics is governed by the symmetry of the highest occupied molecular orbital and that the inclusion of the nuclear motion in the theoretical description generally reduces the intensity of the harmonic radiation. We compare our model with experimental results on N${}_2$ and O${}_2$, and obtain very good agreement.

12 pages, 8 figures, 2 tables; legends revised on Figs. 1,3,4,6 and 7

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• A theory of intense-field dynamic alignment and high harmonic generation from coherently rotating molecules and interpretation of intense-field ultrafast pump-probe experiments
• Strong-field ionization of atoms and molecules: The two-term saddle point method
• Theoretical studies of high-harmonic generation: Effects of symmetry, degeneracy and orientation
• High-order harmonic generation from polyatomic molecules including nuclear motion and a nuclear modes analysis
• High-order harmonic generation from diatomic molecules in elliptically polarized driving fields: a generalized interference condition
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• Interplay of polarization geometry and rotational dynamics in high harmonic generation from coherently rotating linear molecule
• Temporal and spatial interference in molecular above-threshold ionization with elliptically polarized fields
• Influence of asymmetry and nodal planes on high-harmonic generation in heteronuclear molecules
• High-Order Harmonic Generation and Molecular Orbital Tomography: Characteristics of Molecular Recollision Electronic Wave Packets
• Quantum path interferences in high-order harmonic generation from aligned diatomic molecules
• One and two-center processes in high-order harmonic generation in diatomic molecules: influence of the internuclear separation
• Influence of coherent vibronic excitation on the high harmonics generation of diatomic molecules
• Shifting nodal-plane suppressions in high-order harmonic spectra from diatomic molecules in orthogonally polarized driving fields
• Review of the finite difference Hartree-Fock method for atoms and diatomic molecules, and its implementation in the x2dhf program