No Arabic abstract
We study the non-equilibrium structural dynamics of the incommensurate and nearly-commensurate charge-density wave phases in 1T-TaS$_2$. Employing ultrafast low-energy electron diffraction (ULEED) with 1 ps temporal resolution, we investigate the ultrafast quench and recovery of the CDW-coupled periodic lattice distortion. Sequential structural relaxation processes are observed by tracking the intensities of main lattice as well as satellite diffraction peaks as well as the diffuse scattering background. Comparing distinct groups of diffraction peaks, we disentangle the ultrafast quench of the PLD amplitude from phonon-related reductions of the diffraction intensity. Fluence-dependent relaxation cycles reveal a long-lived partial suppression of the order parameter for up to 60 picoseconds, far outlasting the initial amplitude recovery and electron-phonon scattering times. This delayed return to a quasi-thermal level is controlled by lattice thermalization and coincides with the population of zone-center acoustic modes, as evidenced by a structured diffuse background. The long-lived non-equilibrium order parameter suppression suggests hot populations of CDW-coupled lattice modes. Finally, a broadening of the superlattice peaks is observed at high fluences, pointing to a nonlinear generation of phase fluctuations.
The dynamics of the photoinduced commensurate to incommensurate charge density wave (CDW) phase transition in 4Hb-TaSe2 are investigated by femtosecond electron diffraction. In the perturbative regime the CDW reforms on a 150 ps timescale, which is two orders of magnitude slower than in other transition-metal dichalcogenides. We attribute this to a weak coupling between the CDW carrying T-layers and thus demonstrate the importance of three-dimensionality for the existence of CDWs. With increasing optical excitation the phase transition is achieved showing a second order character in contrast to the first order behavior in thermal equilibrium.
We introduce ultrafast low-energy electron diffraction (ULEED) in backscattering for the study of structural dynamics at surfaces. Using a tip-based source of ultrashort electron pulses, we investigate the optically-driven transition between charge-density wave phases at the surface of 1T-TaS2. The large transfer width of the instrument allows us to employ spot-profile analysis, resolving the phase-ordering kinetics in the nascent incommensurate charge-density wave phase. We observe a coarsening that follows a power-law scaling of the correlation length, driven by the annihilation of dislocation-type topological defects of the charge-ordered lattice. Our work opens up the study of a wide class of structural transitions and ordering phenomena at surfaces and in low-dimensional systems.
We report on the ultrafast dynamics of charge order and structural response during the photoinduced suppression of charge and orbital order in a mixed-valence manganite. Employing femtosecond time-resolved resonant x-ray diffraction below and at the Mn K absorption edge, we present a method to disentangle the transient charge order and structural dynamics in thin films of Pr0.5Ca0.5MnO3. Based on the static resonant scattering spectra, we extract the dispersion correction of charge ordered Mn3+ and Mn4+ ions, allowing us to separate the transient contributions of purely charge order from structural contributions to the scattering amplitude after optical excitation. Our finding of a coherent structural mode at around 2.3 THz, which primarily modulates the lattice, but does not strongly affect the charge order, confirms the picture of the charge order being the driving force of the combined charge, orbital and structural transition.
Ground state reconstruction by creation of topological defects in junctions of CDWs is a convenient playground for modern efforts of field-effect transformations in strongly correlated materials with spontaneous symmetry breakings. Being transient, this effect contributes also to another new science of pump-induced phase transitions. We present a dynamical model for behavior of the CDW in restricted geometries of junctions under an applied voltage or a passing current. The model takes into account multiple interacting fields: the amplitude and the phase of the CDW complex order parameter, distributions of the electric field, the density and the current of various normal carriers. A particular challenge was to monitor the local conservation of the condensed and the normal charge densities. That was done easily invoking the chiral invariance and the associated anomaly, but prize is an unconventional Ginsburg-Landau type theory which is not analytic with respect to the order parameter. The numerical modeling poses unusual difficulties but still can demonstrate that vortices are nucleated at the junction boundary when the voltage across, or the current through, exceed a threshold.
Although charge density waves (CDWs) are omnipresent in cuprate high-temperature superconductors, they occur at significantly different wavevectors, confounding efforts to understand their formation mechanism. Here, we use resonant inelastic x-ray scattering to investigate the doping- and temperature-dependent CDW evolution in La2-xBaxCuO4 (x=0.115-0.155). We discovered that the CDW develops in two stages with decreasing temperature. A precursor CDW with quasi-commensurate wavevector emerges first at high-temperature. This doping-independent precursor CDW correlation originates from the CDW phase mode coupled with a phonon and seeds the low-temperature CDW with strongly doping dependent wavevector. Our observation reveals the precursor CDW and its phase mode as the building blocks of the highly intertwined electronic ground state in the cuprates.