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Register a new userUltrafast Dynamics of the Charge Density Wave State in Layered CuxTiSe2
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We report on a transient optical reflectivity study of the charge density wave (CDW) in CuxTiSe2 single crystals. Our measurements reveal that the system undergoes a quantum phase transition at x=0.04 from a strong commensurate CDW (x<0.04) to a soft incommensurate CDW (x>0.04). We find that the cooperative driving mechanisms for the commensurate CDW, the excitonic insulator mechanism and the soft L$_1$$^-$ phonon mode, decouple at x=0.04 with the observed fluctuations in the folded Se-4p band dominating the transition. We also demonstrate a loss of coherence in the A$_{1g}$ phonon with increased copper intercalation of the parent lattice, indicating a loss of long-range lattice order. These findings provide compelling evidence that TiSe2 undergoes a quantum phase transition upon copper intercalation from a state of commensurate charge order to a state with a different symmetry in which the new charge order coexists with the superconducting phase.
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We investigate carrier and collective mode dynamics in 2H-NbSe$_2$ using time-resolved optical pump-probe spectroscopy and compare the results with first-principle calculations. Broadband ultrafast reflectivity studies of 2H-NbSe$_2$ in a wide temperature interval covering the normal, charge density wave (CDW) and superconducting phase were performed. Spectral features observed in the transient reflectivity experiment were associated with specific optical transitions obtained from band structure calculations. Displacive excitation of coherent phonons showed CDW-associated coherent oscillations of the soft phonon mode across the whole spectral range. Temperature evolution of this coherent phonon mode in the low-excitation linear regime shows softening of the mode down to the CDW transition temperature T$_{CDW}$ with subsequent hardening below T$_{CDW}$. The global fit of the broadband probe data reveals four different relaxation times associated with characteristic electron-electron, electron-phonon and phonon-phonon relaxation processes. From first principle calculations of electron-phonon coupling we associate the few picosecond electron-phonon relaxation time $tau_2$ with a specific group of phonons with frequencies around 20 meV. On the other hand, the anomalously long relaxation time of $tau_3$~100 ps is associated with anharmonicity-driven phonon-phonon scattering. All relaxation processes result from anomalies near the second order CDW phase transition that are reflected in the temperature dependencies of the characteristic relaxation times and amplitudes of optical densities. At highest fluences we observe electronic melting of the CDW and disappearance of the mode hardening below T$_{CDW}$.
Low-energy coherent charge-density wave excitations are investigated in blue bronze (K$_{0.3}$MoO$_{3}$) and red bronze (K$_{0.33}$MoO$_{3}$) by femtosecond pump-probe spectroscopy. A linear gapless, acoustic-like dispersion relation is observed for the transverse phasons with a pronounced anisotropy in K$_{0.33}$MoO$_{3}$. The amplitude mode exhibits a weak (optic-like) dispersion relation with a frequency of 1.67 THz at 30 K. Our results show for the first time that the time-resolved optical technique provides momentum resolution of collective excitations in strongly correlated electron systems.Low-energy coherent charge-density wave excitations are investigated in blue bronze (K$_{0.3}$MoO$_{3}$) and red bronze (K$_{0.33}$MoO$_{3}$) by femtosecond pump-probe spectroscopy. A linear gapless, acoustic-like dispersion relation is observed for the transverse phasons with a pronounced anisotropy in K$_{0.33}$MoO$_{3}$. The amplitude mode exhibits a weak (optic-like) dispersion relation with a frequency of 1.67 THz at 30 K. Our results show for the first time that the time-resolved optical technique provides momentum resolution of collective excitations in strongly correlated electron systems.
We report on a thorough optical investigation of BaFe$_2$As$_2$ over a broad spectral range and as a function of temperature, focusing our attention on its spin-density-wave (SDW) phase transition at $T_{SDW}=135$ K. While BaFe$_2$As$_2$ remains metallic at all temperatures, we observe a depletion in the far infrared energy interval of the optical conductivity below $T_{SDW}$, ascribed to the formation of a pseudogap-like feature in the excitation spectrum. This is accompanied by the narrowing of the Drude term consistent with the $dc$ transport results and suggestive of suppression of scattering channels in the SDW state. About 20% of the spectral weight in the far infrared energy interval is affected by the SDW phase transition.
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.
Impurity pinning has long been discussed to have a profound effect on the dynamics of an incommensurate charge density wave (CDW), which would otherwise slide through the lattice without resistance. Here we visualize the impurity pinning evolution of the CDW in ZrTe3 using the variable temperature scanning tunneling microscopy (STM). At low temperatures, we observe a quasi-1D incommensurate CDW modulation moderately correlated to the impurity positions, indicating a weak impurity pinning. As we raise the sample temperature, the CDW modulation gets progressively weakened and distorted, while the correlation with the impurities becomes stronger. Above the CDW transition temperature, short-range modulations persist with the phase almost all pinned by impurities. The evolution from weak to strong impurity pinning through the CDW transition can be understood as a result of losing phase rigidity.
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