We exploit the relationship between high harmonic generation (HHG) and the molecular photorecombination dipole to extract the molecular-frame differential photoionization cross section (PICS) in the extreme ultraviolet (XUV) for molecular nitrogen. A shape resonance and a Cooper-type minimum are reflected in the pump-probe time delay measurements of different harmonic orders, where high-order rotational revivals are observed in N₂. We observe the energy- and angle-dependent Cooper minimum and shape resonance directly in the laboratory-frame HHG yield by achieving a high degree of alignment, [SEE FORMULA IN ABSTRACT cos2 θ] 0.8. The interplay between PICS and rotational revivals is confirmed by simulations using the quantitative rescattering theory. Our method of extracting molecular-frame structural information points the way to similar measurements in more complex molecules.



Keywords and Phrases

Degree Of Alignments; Extreme Ultraviolets; Harmonic Orders; High Harmonic Generation; Molecular Nitrogen; Photoionization Cross Section; Photorecombination; Pump-Probe Time Delay, Electron Resonance; Nitrogen; Photoionization, Harmonic Generation

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Document Type

Article - Journal

Document Version

Final Version

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© 2013 American Physical Society (APS), All rights reserved.

Publication Date

01 Oct 2013

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Physics Commons