Revealing the Cooper minimum of N2 by Molecular Frame High-Harmonic Spectroscopy

Molecular frame high-harmonic spectra of aligned N-2 molecules reveal a Cooper-like minimum. By deconvolving the laboratory frame alignment distribution, what was previously thought to be a maximum of emission along the molecular axis is found to be maxima at 35 degrees off axis, with a spectral minimum on axis. Both of these features are supported by photoionization calculations that underline the relationship between high-harmonic spectroscopy and photoionization measurements. The calculations reveal that the on axis spectral minimum is a Cooper-like minimum that arises from the destructive interference of the p and f partial wave contributions to high-harmonic photorecombination. Features such as Cooper minima and shape resonances are ubiquitous in molecular photoionization or recombination.