Fluctuating charge density waves in a cuprate superconductor

Cuprate materials hosting high-temperature superconductivity (HTS) also exhibit various forms of charge and/or spin ordering whose significance is not fully understood. To date, static charge-density waves (CDWs) have been detected by diffraction probes only at special doping or in an applied external field. However, dynamic CDWs may also be present more broadly and their detection, characterization and relationship with HTS remain open problems. Here, we present a new method, based on ultrafast spectroscopy, to detect the presence and measure the lifetimes of CDW fluctuations in cuprates. In an underdoped La1.9Sr0.1CuO4 film (Tc = 26 K), we observe collective excitations of CDW that persist up to 100 K. This dynamic CDW fluctuates with a characteristic lifetime of 2 ps at T = 5 K which decreases to 0.5 ps at T = 100 K. In contrast, in an optimally doped La1.84Sr0.16CuO4 film (Tc = 38.5 K), we detect no signatures of fluctuating CDWs at any temperature, favoring the competition scenario. This work forges a path for studying fluctuating order parameters in various superconductors and other materials.Comment: 16 pages, 4 figures, accepted to Nature Material

Semiconducting-to-metallic photoconductivity crossover and temperature-dependent Drude weight in graphene

We investigated the transient photoconductivity of graphene at various gate-tuned carrier densities by optical-pump terahertz-probe spectroscopy. We demonstrated that graphene exhibits semiconducting positive photoconductivity near zero carrier density, which crosses over to metallic negative photoconductivity at high carrier density. Our observations are accounted for by considering the interplay between photo-induced changes of both the Drude weight and the carrier scattering rate. Notably, we observed multiple sign changes in the temporal photoconductivity dynamics at low carrier density. This behavior reflects the non-monotonic temperature dependence of the Drude weight, a unique property of massless Dirac fermions

4D visualization of embryonic, structural crystallization by single-pulse microscopy

In many physical and biological systems the transition from an amorphous to ordered native structure involves complex energy landscapes, and understanding such transformations requires not only their thermodynamics but also the structural dynamics during the process. Here, we extend our 4D visualization method with electron imaging to include the study of irreversible processes with a single pulse in the same ultrafast electron microscope (UEM) as used before in the single-electron mode for the study of reversible processes. With this augmentation, we report on the transformation of amorphous to crystalline structure with silicon as an example. A single heating pulse was used to initiate crystallization from the amorphous phase while a single packet of electrons imaged selectively in space the transformation as the structure continuously changes with time. From the evolution of crystallinity in real time and the changes in morphology, for nanosecond and femtosecond pulse heating, we describe two types of processes, one that occurs at early time and involves a nondiffusive motion and another that takes place on a longer time scale. Similar mechanisms of two distinct time scales may perhaps be important in biomolecular folding

Nonlinear optical probe of tunable surface electrons on a topological insulator

We use ultrafast laser pulses to experimentally demonstrate that the second-order optical response of bulk single crystals of the topological insulator Bi$_2$Se$_3$ is sensitive to its surface electrons. By performing surface doping dependence measurements as a function of photon polarization and sample orientation we show that second harmonic generation can simultaneously probe both the surface crystalline structure and the surface charge of Bi$_2$Se$_3$. Furthermore, we find that second harmonic generation using circularly polarized photons reveals the time-reversal symmetry properties of the system and is surprisingly robust against surface charging, which makes it a promising tool for spectroscopic studies of topological surfaces and buried interfaces

Invariant quantum discord in qubit-qutrit systems under local dephasing

We investigate the dynamics of quantum discord and entanglement for a class of mixed qubit-qutrit states assuming that only the qutrit is under the action of a dephasing channel. We demonstrate that even though the entanglement in the qubit-qutrit state disappears in a finite time interval, partial coherence left in the system enables quantum discord to remain invariant throughout the whole time evolution

Real time observation of cuprates structural dynamics by Ultrafast Electron Crystallography

The phonon-mediated attractive interaction between carriers leads to the Cooper pair formation in conventional superconductors. Despite decades of research, the glue holding Cooper pairs in high-temperature superconducting cuprates is still controversial, and the same is true as for the relative involvement of structural and electronic degrees of freedom. Ultrafast electron crystallography (UEC) offers, through observation of spatio-temporally resolved diffraction, the means for determining structural dynamics and the possible role of electron-lattice interaction. A polarized femtosecond (fs) laser pulse excites the charge carriers, which relax through electron-electron and electron-phonon coupling, and the consequential structural distortion is followed diffracting fs electron pulses. In this review, the recent findings obtained on cuprates are summarized. In particular, we discuss the strength and symmetry of the directional electron-phonon coupling in Bi2Sr2CaCu2O8+\delta (BSCCO), as well as the c-axis structural instability induced by near-infrared pulses in La2CuO4 (LCO). The theoretical implications of these results are discussed with focus on the possibility of charge stripes being significant in accounting for the polarization anisotropy of BSCCO, and cohesion energy (Madelung) calculations being descriptive of the c-axis instability in LCO

Observation of a metal-to-insulator transition with both Mott-Hubbard and Slater characteristics in Sr_2IrO_4 from time-resolved photocarrier dynamics

We perform a time-resolved optical study of Sr_2IrO_4 to understand the influence of magnetic ordering on the low energy electronic structure of a strongly spin-orbit coupled J_(eff) = 1/2 Mott insulator. By studying the recovery dynamics of photoexcited carriers, we find that upon cooling through the Néel temperature T_N the system evolves continuously from a metal-like phase with fast (∼50 fs) and excitation density independent relaxation dynamics to a gapped phase characterized by slower (∼500 fs) excitation density-dependent bimolecular recombination dynamics, which is a hallmark of a Slater-type metal-to-insulator transition. However our data indicate that the high energy reflectivity associated with optical transitions into the unoccupied J_(eff) = 1/2 band undergoes the sharpest upturn at TN, which is consistent with a Mott-Hubbard type metal-to-insulator transition involving spectral weight transfer into an upper Hubbard band. These findings show Sr_2IrO_4 to be a unique system in which Slater- and Mott-Hubbard-type behaviors coexist and naturally explain the absence of anomalies at T_N in transport and thermodynamic measurements