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High-order harmonic generation (HHG) in aligned linear molecules can offervaluable information about strong-field interactions in lower-lying molecularorbitals, but extracting this information is difficult for three-dimensionalmolecular geometries. Our measurements of the asymmetric top SO2 show largeaxis dependencies, which change with harmonic order. The analysis shows thatthese spectral features must be due to field ionization and recombination frommultiple orbitals during HHG. We expect that HHG can probe orbital dependenciesusing this approach for a broad class of asymmetric-top molecules.

Multiple orbital contributions to molecular high-harmonic generation in an asymmetric top