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    Tracking ultrafast solid-state dynamics using high harmonic spectroscopy
    (College Park, MD : APS, 2021) Bionta, Mina R.; Haddad, Elissa; Leblanc, Adrien; Gruson, Vincent; Lassonde, Philippe; Ibrahim, Heide; Chaillou, Jérémie; Émond, Nicolas; Otto, Martin R.; Siwick, Bradley J.; Chaker, Mohamed; Légaré, François
    WWe 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 insulator-to-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.
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    Ultrafast nonlocal collective dynamics of Kane plasmon-polaritons in a narrow-gap semiconductor
    (Washington : American Association for the Advancement of Science (A A A S), 2019) Charnukha, A.; Sternbach, A.; Stinson, H.T.; Schlereth, R.; Brüne, C.; Molenkamp, L.W.; Basov, D.N.
    The observation of ultrarelativistic fermions in condensed-matter systems has uncovered a cornucopia of novel phenomenology as well as a potential for effective ultrafast light engineering of new states of matter. While the nonequilibrium properties of two- and three-dimensional (2D and 3D) hexagonal crystals have been studied extensively, our understanding of the photoinduced dynamics in 3D single-valley ultrarelativistic materials is, unexpectedly, lacking. Here, we use ultrafast scanning near-field optical spectroscopy to access and control nonequilibrium large-momentum plasmon-polaritons in thin films of a prototypical narrow-bandgap semiconductor Hg0.81Cd0.19Te. We demonstrate that these collective excitations exhibit distinctly nonclassical scaling with electron density characteristic of the ultrarelativistic Kane regime and experience ultrafast initial relaxation followed by a long-lived highly coherent state. Our observation and ultrafast control of Kane plasmon-polaritons in a semiconducting material using light sources in the standard telecommunications fiber-optics window open a new avenue toward high-bandwidth coherent information processing in next-generation plasmonic circuits.