Tracking ultrafast solid-state dynamics using high harmonic spectroscopy
Mina R. Bionta, Elissa Haddad, Adrien Leblanc, Vincent Gruson, Philippe Lassonde, Heide Ibrahim, Jérémie Chaillou, Nicolas Émond, Martin R. Otto, Álvaro Jiménez-Galán, Rui E. F. Silva, Misha Ivanov, Bradley J. Siwick, Mohamed Chaker, François Légaré
Abstract
We establish time-resolved high harmonic generation (tr-HHG) as a powerful spectroscopy method for tracking photoinduced dynamics in strongly correlated materials through a detailed investigation of the insulatorto-metal phase transitions in vanadium dioxide. We benchmark the 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 of 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.