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Register a new userUltrafast dynamics of charge density waves in 4Hb-TaSe2 probed by femtosecond electron diffraction
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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.
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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.
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 study of a magnetic dislocation in pure chromium. Coherent x-ray diffraction profiles obtained on the incommensurate Spin Density Wave (SDW) reflection are consistent with the presence of a dislocation of the magnetic order, embedded at a few micrometers from the surface of the sample. Beyond the specific case of magnetic dislocations in chromium, this work may open up a new method for the study of magnetic defects embedded in the bulk.
The charge density wave (CDW) state in van der Waals systems shows interesting scaling phenomena as the number of layers can significantly affect the CDW transition temperature, $T_{CDW}$. However, it is often difficult to use conventional methods to study the phase transition in these systems due to their small size and sensitivity to degradation. Degradation is an important parameter which has been shown to greatly influence the superconductivity in layered systems. Since the CDW state competes with the onset of superconductivity, it is expected that $T_{CDW}$ will also be affected by the degradation. Here, we probe the CDW phase transition by the mechanical resonances of suspended 2H-TaS2 and 2H-TaSe2 membranes and study the effect of disorder on the CDW state. Pristine flakes show the transition near the reported values of 75 K and 122 K respectively. We then study the effect of degradation on 2H-TaS2 which displays an enhancement of $T_{CDW}$ up to 129 K after degradation in ambient air. Finally, we study a sample with local degradation and observe that multiple phase transitions occur at 87 K, 103 K and 118 K with a hysteresis in temperature in the same membrane. The observed spatial variations in the Raman spectra suggest that variations in crystal structure cause domains with different transition temperatures which could result in the hysteresis. This work shows the potential of using nanomechanical resonance to characterize the CDW in suspended 2D materials and demonstrate that degradation can have a large effect on transition temperatures.
We investigate the thermal-driven charge density wave (CDW) transition of two cubic superconducting intermetallic systems Lu(Pt1-xPdx)2In and (Sr1-xCax)3Ir4Sn13 by means of x-ray diffraction technique. A detailed analysis of the CDW modulation superlattice peaks as function of temperature is performed for both systems as the CDW transition temperature T_CDW is suppressed to zero by an non-thermal control parameter. Our results indicate an interesting crossover of the classical thermal-driven CDW order parameter critical exponent from a three-dimensional universality class to a mean-field tendency, as T_CDW vanishes. Such behavior might be associated with presence of quantum fluctuations which influences the classical second-order phase transition, strongly suggesting the presence of a quantum critical point (QCP) at T_CDW = 0. This also provides experimental evidence that the effective dimensionality exceeds its upper critical dimension due to a quantum phase transition.
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