Polarization-state-resolved high-harmonic spectroscopy of solids

Attosecond metrology sensitive to sub-optical-cycle electronic and structural dynamics is opening up new avenues for ultrafast spectroscopy of condensed matter. Using intense lightwaves to precisely control the extremely fast carrier dynamics in crystals holds great promise for next-generation electronics and devices operating at petahertz bandwidth. The carrier dynamics can produce high-order harmonics of the driving light field extending up into the extreme-ultraviolet region. Here, we introduce polarization-state-resolved high-harmonic spectroscopy of solids, which provides deeper insights into both electronic and structural dynamics occuring within a single cycle of light. Performing high-harmonic generation measurements from silicon and quartz samples, we demonstrate that the polarization states of high-order harmonics emitted from solids are not only determined by crystal symmetries, but can be dynamically controlled, as a consequence of the intertwined interband and intraband electronic dynamics, responsible for the harmonic generation. We exploit this symmetry-dynamics duality to efficiently generate circularly polarized harmonics from elliptically polarized driver pulses. Our experimental results are supported by ab-initio simulations, providing clear evidence for the microscopic origin of the phenomenon. This spectroscopy technique might find important applications in future studies of novel quantum materials such as strongly correlated materials. Compact sources of bright circularly polarized harmonics in the extreme-ultraviolet regime will advance our tools for the spectroscopy of chiral systems, magnetic materials, and 2D materials with valley selectivity.