Revealing the Interplay between Strong Field Selection Rules and Crystal Symmetries

Symmetries are ubiquitous in condensed matter physics, playing an important role in the appearance of different phases of matter. Nonlinear light matter interactions serve as a coherent probe for resolving symmetries and symmetry breaking via their link to selection rules of the interaction. In the extreme nonlinear regime, high harmonic generation (HHG) spectroscopy offers a unique spectroscopic approach to study this link, probing the crystal spatial properties with high sensitivity while opening new paths for selection rules in the XUV regime. In this Letter we establish an advanced HHG polarimetry scheme, driven by a multicolor strong laser field, to observe the structural symmetries of solids and their interplay with the HHG selection rules. By controlling the crystal symmetries, we resolve nontrivial polarization states associated with new spectral features in the HHG spectrum. Our scheme opens new opportunities in resolving the symmetries of quantum materials, as well as ultrafast light driven symmetries in condensed matter systems.