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Tracking ultrafast solid-state dynamics using high harmonic spectroscopy

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posted on 2023-11-30, 19:36 authored by Mina R. Bionta, Elissa Haddad, Adrien Leblanc, Vincent Gruson, Philippe Lassonde, Heide Ibrahim, Jérémie Chaillou, Nicolas Émond, Martin R. Otto, Bradley J. Siwick, Mohamed Chaker, François Légaré
We establish time-resolved high harmonic generation (tr-HHG) as a powerful spectroscopy for photoinduced dynamics in strongly correlated materials through a detailed investigation of the insulator-to-metal transitions in vanadium dioxide. We benchmark our technique by comparing our measurements to established momentum-resolved ultrafast electron diffraction, and theoretical density functional calculations. Tr-HHG allows distinguishing of individual dynamic channels, including a transition to a thermodynamically hidden phase. In addition, the HHG yield is shown to be modulated at a frequency characteristic of a coherent phonon in the equilibrium monoclinic phase over a wide range of excitation fluences. These results demonstrate that tr-HHG is capable of tracking complex dynamics in solids through its sensitivity to the band structure.

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