Abstract
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 fast carrier dynamics in crystals holds great promise for next-generation petahertz electronics and devices. The carrier dynamics can produce high-order harmonics of the driving 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 sub-cycle dynamics. Performing high-harmonic generation measurements from silicon and quartz, we demonstrate that the polarization states of the harmonics are not only determined by crystal symmetries, but can be dynamically controlled, as a consequence of the intertwined interband and intraband electronic dynamics. We exploit this symmetry-dynamics duality to efficiently generate coherent circularly polarized harmonics from elliptically polarized pulses. Our experimental results are supported by ab-initio simulations, providing evidence for the microscopic origin of the phenomenon.
Highlights
Attosecond metrology sensitive to sub-optical-cycle electronic and structural dynamics is opening up new avenues for ultrafast spectroscopy of condensed matter
We found that both crystal symmetry and the nonperturbative coupled interband and intraband dynamics underlying harmonic emission play decisive roles in the polarization states of the emitted harmonics
We have elucidated this duality between symmetry and dynamics in experiments on high-harmonic generation from silicon and quartz accompanied by ab-initio time-dependent density functional theory (TDDFT) simulations
Summary
Attosecond metrology sensitive to sub-optical-cycle electronic and structural dynamics is opening up new avenues for ultrafast spectroscopy of condensed matter. Performing highharmonic generation measurements from silicon and quartz, we demonstrate that the polarization states of the harmonics are determined by crystal symmetries, but can be dynamically controlled, as a consequence of the intertwined interband and intraband electronic dynamics. Adapting attosecond metrology techniques[2] to observe and control the fastest electronic dynamics in the plethora of known solids and novel quantum materials[3] is very promising for studying correlated electronic dynamics (e.g., excitonic effects, screening) on atomic length and time scales, thereby potentially impacting future technologies such as emerging petahertz electronic signal processing[2,4] or strong-field optoelectronics[5,6]. That work predicted that different harmonics react differently to the driver ellipticity, as they can either originate mainly from intraband contributions or from coupled interband and intraband dynamics[14]
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