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High-harmonic generation was used to probe the spectral intensity and phase of the recombination-dipole matrix element of methyl chloride (CH3Cl), revealing a Cooper minimum (CM) analogous to the 3p CM previously reported in argon. The CM structure altered the spectral response and group delay (GD) of the emitted harmonics, and was revealed only through careful removal of all additional contributors to the GD. In characterizing the GD dispersion, also known as the “attochirp” we additionally present the most complete validation to date of the commonly used strong-field approximation for calculating the GD, demonstrating the correct intensity scaling and extending its usefulness to simple molecules.

Full Characterization of a Molecular Cooper Minimum Using High-Harmonic Spectroscopy