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- ItemCoherent Rabi dynamics of a superradiant spin ensemble in a microwave cavity(College Park, Md. : APS, 2017) Rose, B.C.; Tyryshkin, A.M.; Riemann, H.; Abrosimov, N.V.; Becker, P.; Pohl, H.-J.; Thewalt, M.L.W.; Itoh, K.M.; Lyon, S.A.We achieve the strong-coupling regime between an ensemble of phosphorus donor spins in a highly enriched 28Si crystal and a 3D dielectric resonator. Spins are polarized beyond Boltzmann equilibrium using spin-selective optical excitation of the no-phonon bound exciton transition resulting in N=3.6×1013 unpaired spins in the ensemble. We observe a normal mode splitting of the spin-ensemble–cavity polariton resonances of 2g√N=580 kHz (where each spin is coupled with strength g) in a cavity with a quality factor of 75 000 (γ≪κ≈60 kHz, where γ and κ are the spin dephasing and cavity loss rates, respectively). The spin ensemble has a long dephasing time (T∗2=9 μs) providing a wide window for viewing the dynamics of the coupled spin-ensemble–cavity system. The free-induction decay shows up to a dozen collapses and revivals revealing a coherent exchange of excitations between the superradiant state of the spin ensemble and the cavity at the rate g√N. The ensemble is found to evolve as a single large pseudospin according to the Tavis-Cummings model due to minimal inhomogeneous broadening and uniform spin-cavity coupling. We demonstrate independent control of the total spin and the initial Z projection of the psuedospin using optical excitation and microwave manipulation, respectively. We vary the microwave excitation power to rotate the pseudospin on the Bloch sphere and observe a long delay in the onset of the superradiant emission as the pseudospin approaches full inversion. This delay is accompanied by an abrupt π-phase shift in the peusdospin microwave emission. The scaling of this delay with the initial angle and the sudden phase shift are explained by the Tavis-Cummings model.
- ItemCoherent control of the photoinduced transition in a strongly correlated material(College Park, MD : APS, 2022) Molinero, Eduardo B.; Silva, Rui E. F.The use of intense tailored light fields is the perfect tool to achieve ultrafast control of electronic properties in quantum materials. Among them, Mott insulators are materials in which strong electron-electron interactions drive the material into an insulating phase. When shining a Mott insulator with a strong laser pulse, the electric field may induce the creation of doublon-hole pairs, triggering a photoinduced transition into a metallic state. In this paper, we take advantage of the threshold character of this photoinduced transition and we propose a setup that consists of a midinfrared laser pulse and a train of short pulses separated by a half period of the midinfrared with alternating phases. By varying the time delay between the two pulses and the internal carrier envelope phase of the short pulses, we achieve control of the phase transition, which leaves its fingerprint at its high harmonic spectrum.
- ItemTracking 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, FrançoisWWe 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.