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Register a new userProbing the coupling between a doublon excitation and the charge-density wave in TaS2 by ultrafast optical spectroscopy
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Recently, the switching between the different charge-ordered phases of 1T-TaS2 has been probed by ultrafast techniques, revealing unexpected phenomena such as hidden metastable states and peculiar photoexcited charge patterns. Here, we apply broadband pump-probe spectroscopy with varying excitation energy to study the ultrafast optical properties of 1T-TaS2 in the visible regime. By scanning the excitation energy in the near-IR region we unravel the coupling between different charge excitations and the low-lying charge-density wave state. We find that the amplitude mode of the charge-density wave exhibits strong coupling to a long-lived doublon state that is photoinduced in the center of the star-shaped charge-ordered Ta clusters by the near-IR optical excitation.
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Electron-phonon-driven charge density waves can in some circumstances allow electronic correlations to become predominant, driving a system into a Mott insulating state. New insights into both the Mott state and preceding charge density wave may result from observations of the coupled dynamics of their underlying degrees of freedom. Here, tunneling injection of single electrons into the upper Hubbard band of the Mott charge-density-wave material 1T-TaS2 reveals extraordinarily narrow electronic excitations which couple to amplitude mode phonons associated with the charge density waves periodic lattice distortion. This gives a vivid microscopic view of the interplay between excitations of the Mott state and the lattice dynamics of its charge density wave precursor.
Femtosecond time-resolved core-level photoemission spectroscopy with a free-electron laser is used to measure the atomic-site specific charge-order dynamics in the charge-density-wave/Mott insulator 1T-TaS2. After strong photoexcitation, a prompt loss of charge order and subsequent fast equilibration dynamics of the electron-lattice system are observed. On the time scale of electron-phonon thermalization, about 1 ps, the system is driven across a phase transition from a long-range charge ordered state to a quasi-equilibrium state with domain-like short-range charge and lattice order. The experiment opens the way to study the nonequilibrium dynamics of condensed matter systems with full elemental, chemical, and atomic site selectivity.
We report on a Raman scattering investigation of the charge-density-wave (CDW), quasi two-dimensional rare-earth tri-tellurides $R$Te$_3$ ($R$= La, Ce, Pr, Nd, Sm, Gd and Dy) at ambient pressure, and of LaTe$_3$ and CeTe$_3$ under externally applied pressure. The observed phonon peaks can be ascribed to the Raman active modes for both the undistorted as well as the distorted lattice in the CDW state by means of a first principles calculation. The latter also predicts the Kohn anomaly in the phonon dispersion, driving the CDW transition. The integrated intensity of the two most prominent modes scales as a characteristic power of the CDW-gap amplitude upon compressing the lattice, which provides clear evidence for the tight coupling between the CDW condensate and the vibrational modes.
We report the ultrafast optical pump-probe spectroscopy measurements on the recently discovered quantum critical ferromagnet CeRh$_6$Ge$_4$. Our experimental results reveal the two-stage development of the hybridization between localized $f$ moments and conduction electrons with lowering temperature, as evidenced by (1) the presence of hybridization fluctuation for temperatures from $sim$85 K ($T^*$) to $sim$140 K ($T^dagger$), and (2) the emergence of collective hybridization below the coherence temperature, $T^*$, marked by the opening of an indirect gap of 2$Delta$ $approx$12 meV. We also observe three coherent phonon modes being softened anomalously below $T^*$, reflecting directly their coupling with the emergent coherent heavy electrons. Our findings establish the universal nature of the hybridization process in different heavy fermion systems.
We investigate the quasiparticle dynamics in the prototype heavy fermion CeCoIn$_5$ using ultrafast optical pump-probe spectroscopy. Our results indicate that this material system undergoes hybridization fluctuations before full establishment of the heavy electron coherence, as the temperature decreases from $sim$120 K ($T^dagger$) to $sim$55 K ($T^*$ ). We reveal that the observed anomalous phonon softening and damping reduction below $T^*$ are directly associated with opening of an indirect hybridization gap. We also discover a distinct collective mode with an energy of $sim$8 meV, which may be the experimental evidence of the predicted unconventional density wave. Our observations provide critical informations for understanding the hybridization dynamics in heavy fermion materials.
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