Spin angular momentum and tunable polarization in high-harmonic generation

The roles of energy, momentum and orbital angular momentum conservation in high-harmonic generation were studied in the past. Here, we explore the role of spin angular momentum in high-harmonic generation by experimentally generating high harmonics of bichromatic elliptically polarized pump beams that interact with isotropic media. We explain qualitatively many observed intricate selection rules with a model that includes spin conservation in the conversion of many pump photons into a single photon. However, we also observe unequivocal deviations from this model, indicating that emission of an elliptically polarized high-energy photon is accompanied by an additional excitation (radiative or electronic). The presented results are also important for applications, because our system exhibits full control over the polarization of the harmonics, from circular through elliptical to linear polarization, without compromising the efficiency of the process. This work paves the way for a broad range of applications with high-harmonic generation, including ultrafast circular dichroism of molecules and magnetic materials.