Uncovering Multiple Orbitals Influence in High Harmonic Generation from Aligned N₂

Abstract

Recent measurements on high-order harmonic generation (HHG) from N₂ aligned perpendicular to the driving laser polarization (B K McFarland et al 2008 Science 322 1232) have shown a maximum at the rotational half-revival. This has been interpreted as the signature of the HHG contribution from the molecular orbital just below the highest occupied molecular orbital (HOMO). By using the recently developed quantitative rescattering theory combined with accurate photoionization transition dipoles, we show that the maximum at the rotational half-revival is indeed associated with the HOMO-1 contribution. Our results also show that the HOMO-1 contribution becomes increasingly more important near the HHG cutoff and therefore depends on the laser intensity.

Department(s)

Physics

Keywords and Phrases

High Harmonic Generation; High Order Harmonic Generation; Highest Occupied Molecular Orbital; Laser Intensities; Laser Polarization; Orbitals; Photoionization Transitions; Rescattering, Molecular Modeling; Molecular Orbitals, Harmonic Generation

International Standard Serial Number (ISSN)

0953-4075

Document Type

Article - Journal

Document Version

Citation

File Type

text

Language(s)

English

Rights

© 2009 IOP Publishing Ltd., All rights reserved.

Publication Date

01 Oct 2009

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