High harmonic generation (HHG) is a unique and useful process in which infrared or visible radiation is frequency up-converted into the extreme ultraviolet and x-ray spectral regions. As a parametric process, high harmonic generation should conserve the radiation energy, momentum and angular momentum. Indeed, conservation of energy and momentum have been demonstrated. Angular momentum of optical beams can be divided into two components: orbital and spin (polarization). Orbital angular momentum is assumed to be conserved and recently observed deviations were attributed to propagation effects. On the other hand, conservation of spin angular momentum has thus far never been studied, neither experimentally nor theoretically.
We present the first study on the role of spin angular momentum in extreme nonlinear optics by experimentally generating high harmonics of bi-chromatic elliptically-polarized pump beams that interact with isotropic media. While observing that the selection rules qualitatively correspond to spin conservation, we unequivocally find that the process of converting pump photons into a single high-energy photon does not conserve angular momentum, i.e. this process is not self-contained. In one regime, we numerically find that this major fundamental discrepancy can be explained if the harmonic photons are emitted in pairs. The results presented here, apart from exploring the very foundations of HHG, are also important for a variety of applications – as our system exhibits full control over the harmonics polarization, from circular through elliptical to linear polarization, without comprising the efficiency of the process. This work paves the way for a broad range of applications with HHG, from ultrafast circular dichroism to attosecond quantum optics.