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 fast carrier dynamics in crystals holds great promise for next-generation petahertz elect...

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Bibliographic Details
Published in:Nature communications 2019-03, Vol.10 (1), p.1319-1319, Article 1319
Main Authors: Klemke, N., Tancogne-Dejean, N., Rossi, G. M., Yang, Y., Scheiba, F., Mainz, R. E., Di Sciacca, G., Rubio, A., Kärtner, F. X., Mücke, O. D.
Format: Article
Language:English
Subjects:
140/125
639/301/119
639/766/400/3923
Circular polarization
Crystals
Dynamics
Electronic devices
Harmonic generations
Humanities and Social Sciences
multidisciplinary
Polarization
Science
Science (multidisciplinary)
Solids
Spectroscopy
Spectrum analysis
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Summary: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. High-harmonic generation in solids is related to the carrier dynamics and can be used to probe dynamic processes. Here, Klemke et al. show that the polarization states of high harmonics generated from silicon and quartz are determined by the crystal symmetries but can also be dynamically controlled.
ISSN:2041-1723
2041-1723
DOI:10.1038/s41467-019-09328-1