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Superconductivity and charge density waves (CDW) are competitive, yet coexisting orders in cuprate superconductors. To understand their microscopic interdependence, a probe capable of discerning their interaction on its natural length and time scales is necessary. We use ultrafast resonant soft x-ray scattering to track the transient evolution of CDW correlations in YBa$_{2}$Cu$_{3}$O$_{6+x}$ following the quench of superconductivity by an infrared laser pulse. We observe a non-thermal response of the CDW order characterized by a near doubling of the correlation length within $\approx$ 1 picosecond of the superconducting quench. Our results are consistent with a model in which the interaction between superconductivity and CDW manifests inhomogeneously through disruption of spatial coherence, with superconductivity playing the dominant role in stabilizing CDW topological defects, such as discommensurations., Comment: Accepted version. 34 pages, 11 figures, Main text and Supplementary Materials

Resonant inelastic x-ray scattering (RIXS) provides remarkable opportunities to interrogate ultrafast dynamics in liquids. Here we use RIXS to study the fundamentally and practically important hydroxyl radical in liquid water, OH(aq). Impulsive ionization of pure liquid water produced a short-lived population of OH(aq), which was probed using femtosecond x-rays from an x-ray free-electron laser. We find that RIXS reveals localized electronic transitions that are masked in the ultraviolet absorption spectrum by strong charge-transfer transitions -- thus providing a means to investigate the evolving electronic structure and reactivity of the hydroxyl radical in aqueous and heterogeneous environments. First-principles calculations provide interpretation of the main spectral features., Comment: 40 pages, 10 figures

The condensation of an electron superfluid from a conventional metallic state at a critical temperature $T_c$ is described well by the BCS theory. In the underdoped copper-oxides, high-temperature superconductivity condenses instead from a nonconventional metallic "pseudogap" phase that exhibits a variety of non-Fermi liquid properties. Recently, it has become clear that a charge density wave (CDW) phase exists within the pseudogap regime, appearing at a temperature $T_{CDW}$ just above $T_c$. The near coincidence of $T_c$ and $T_{CDW}$, as well the coexistence and competition of CDW and superconducting order below $T_c$, suggests that they are intimately related. Here we show that the condensation of the superfluid from this unconventional precursor is reflected in deviations from the predictions of BSC theory regarding the recombination rate of quasiparticles. We report a detailed investigation of the quasiparticle (QP) recombination lifetime, $\tau_{qp}$, as a function of temperature and magnetic field in underdoped HgBa$_{2}$CuO$_{4+\delta}$ (Hg-1201) and YBa$_{2}$Cu$_{3}$O$_{6+x}$ (YBCO) single crystals by ultrafast time-resolved reflectivity. We find that $\tau_{qp}(T)$ exhibits a local maximum in a small temperature window near $T_c$ that is prominent in underdoped samples with coexisting charge order and vanishes with application of a small magnetic field. We explain this unusual, non-BCS behavior by positing that $T_c$ marks a transition from phase-fluctuating SC/CDW composite order above to a SC/CDW condensate below. Our results suggest that the superfluid in underdoped cuprates is a condensate of coherently-mixed particle-particle and particle-hole pairs.

We report equilibrium and nonequilibrium optical measurements on the recently synthesized "harmonic" honeycomb iridate \gamma-Li$_2$IrO$_3$ (LIO), as well as the layered honeycomb iridate Na$_2$IrO$_3$ (NIO). Using Fourier transform infrared microscopy we performed reflectance measurements on LIO, from which we obtained the optical conductivity below 2 eV. In addition we measured the photoinduced changed in reflectance, \Delta R, as a function of time, t, temperature, T, and probe field polarization in both LIO and NIO. In LIO, \Delta R(t,T) is anisotropic and comprised of three T dependent components. Two of these components are related to the onset of magnetic order and the third is related to a photoinduced population of metastable electronic excited states. In NIO, \Delta R(t,T) has a single T dependent component that is strikingly similar to the electronic excitation component of \Delta R in LIO. Through analysis and comparison of \Delta R(t,T) for two compounds, we extract information on the onset of magnetic correlations at and above the transition temperature in LIO, the bare spin-flip scattering rate in equilibrium, the lifetime of low-lying quasiparticle excitations, and the polarization dependence of optical transitions that are sensitive to magnetic order.

We report the observation of coherent oscillations associated with charge density wave (CDW) order in the underdoped cuprate superconductor YBa2Cu3O6+x by time-resolved optical reflectivity. Oscillations with frequency 1.87 THz onset at approximately 105 K and 130 K for dopings of x = 0.67 (ortho-VIII) and x = 0.75 (ortho-III), respectively. Upon cooling below the superconducting critical temperature (T_c), the oscillation amplitude is enhanced, the phase shifts by \pi, and the frequency softens by \delta \nu / \nu~7%. A bi-quadratically coupled Landau-Ginzburg model qualitatively describes this behavior as arising from competition between superconducting and CDW orders.

We use phase-resolved transient grating spectroscopy to measure the propagation of spin helices in a high mobility $n$-GaAs/AlGaAs quantum well with an applied in-plane electric field. At relatively low fields helical modes crossover from overdamped excitations where the spin-precession period exceeds the spin lifetime, to a regime of coherent propagation where several spin-precession periods can be observed. We demonstrate that the envelope of a spin polarization packet reaches a current-driven velocity of 10$^7$ cm s$^{-1}$ in an applied field of 70 V cm$^{-1}$.

Controlling the flow of electrons by manipulation of their spin is a key to the development of spin-based electronics. While recent demonstrations of electrical-gate control in spin-transistor configurations show great promise, operation at room temperature remains elusive. Further progress requires a deeper understanding of the propagation of spin polarization, particularly in the high mobility semiconductors used for devices. Here we report the application of Doppler velocimetry to resolve the motion of spin-polarized electrons in GaAs quantum wells driven by a drifting Fermi sea. We find that the spin mobility tracks the high electron mobility precisely as a function of T. However, we also observe that the coherent precession of spins driven by spin-orbit interaction, which is essential for the operation of a broad class of spin logic devices, breaks down at temperatures above 150 K for reasons that are not understood theoretically.

We study the magnetic excitations of itinerant helimagnets by applying time-resolved optical spectroscopy to Fe0.8Co0.2Si. Optically excited oscillations of the magnetization in the helical state are found to disperse to lower frequency as the applied magnetic field is increased; the fingerprint of collective modes unique to helimagnets, known as helimagnons. The use of time-resolved spectroscopy allows us to address the fundamental magnetic relaxation processes by directly measuring the Gilbert damping, revealing the versatility of spin dynamics in chiral magnets. (*These authors contributed equally to this work)

We use coherent pump-probe spectroscopy to measure the photoinduced reflectivity \DeltaR, and complex dielectric function, {\delta}\in, of the electron-doped cuprate superconductor Nd_{2-x}Ce_xCuO_{4+\delta} at a value of x near optimal doping, as a function of time, temperature, and laser fluence. We observe the onset of a negative \DeltaR at T=85 K, above the superconducting transition temperature, T_c, of 23 K, that exhibits a form of scaling consistent with critical fluctuations in the time domain. A positive \Delta R onsets at T_c that we associate with superconducting order. We find that the two signals are strongly coupled below T_c, in a manner that suggests a repulsive interaction between superconductivity and antiferromagnetic correlations.

We use phase-resolved transient grating spectroscopy to measure the drift and diffusion of electron-hole density waves in a semiconductor quantum well. The unique aspects of this optical probe allow us to determine the frictional force between a two-dimensional Fermi liquid of electrons and a dilute gas of holes. Knowledge of electron-hole friction enables prediction of ambipolar dynamics in high-mobility electron systems., Comment: to appear in PRL

In this supporting material for the main paper (the preceding submission), we show, in addition to the related information for the experiments, additional discussion that cannot fit in the main paper (due to the space constraint). It includes further discussion about our experimental observations, wider implications of our main findings with various reported candidates for the pseudogap order, and a simple mean-field argument that favors interpretations based on a finite-Q order (density wave) for the pseudogap seen by ARPES (whether "the pseudogap order" is a single order or contains multiple ingredients, is an independent, open issue). We also include a detailed simulation section, in which we model different candidates (various density wave/nematic order) for the pseudogap order in simple forms using a mean-field approach, and discuss their partial success as well as limitations in describing the experimental observations. These simulations are based on a tight-binding model with parameters fitted globally (and reasonably well) to the experimental band dispersions (by tracking the maximum of the energy distribution curve), which could be useful for further theoretical explorations on this issue.

Using low-photon energy angle-resolved photoemission (ARPES), we study the low-energy dispersion along the nodal (pi, pi) direction in Bi(2)Sr(2)CaCu(2)O(8+delta) (Bi2212) as a function of temperature. Less than 10 meV below the Fermi energy, the high-resolution data reveals a novel "kink"-like feature in the real part of the electron self-energy that is distinct from the larger well-known kink roughly 70 meV below E_F. This new kink is strongest below the superconducting critical temperature and weakens substantially as the temperature is raised. A corollary of this finding is that the Fermi velocity, as measured over this energy range, varies rapidly with temperature - increasing by almost 30% from 70 to 110 K., Comment: 5 pages, 3 figures, citation added, submitted to Phys. Rev. Lett

Anderson has recently proposed a theory of the strange metal state above Tc in the high Tc superconductors. [arXiv:cond-mat/0512471] It is based on the idea that the unusual transport properties and spectral functions are caused by the strong Mott- Hubbard interactions and can be computed by using the formal apparatus of Gutzwiller projection. In ref. 1 Anderson computed only the tunneling spectrum and the power-law exponent of the infrared conductivity. He had calculated the energy distribution curves (EDCs) in angle resolved photoemission spectroscopy (ARPES) but was discouraged when these differed radically from the best ARPES measurements available at the time, and did not include them. In this letter we compare the spectral functions computed within this model to the novel laser-ARPES data of the Dessau group.These are found to capture the shape of the experimental EDCs with unprecedented accuracy and in principle have only one free parameter.

A laser-based angle resolved photoemission (APRES) system utilizing 6 eV photons from the fourth harmonic of a mode-locked Ti:sapphire oscillator is described. This light source greatly increases the momentum resolution and photoelectron count rate, while reducing extrinsic background and surface sensitivity relative to higher energy light sources. In this review, the optical system is described, and special experimental considerations for low-energy ARPES are discussed. The calibration of the hemispherical electron analyzer for good low-energy angle-mode performance is also described. Finally, data from the heavily studied high T_c superconductor Bi2Sr2CaCu2O8+\delta (Bi2212) is compared to the results from higher photon energies., Comment: Please download final version from Journal-Ref

A new low photon energy regime of angle resolved photoemission spectroscopy is accessed with lasers and used to study the superconductor Bi2Sr2CaCu2O8+delta. The low energy increases bulk sensitivity, reduces background, and improves resolution. With this we observe spectral peaks which are sharp on the scale of their binding energy - the clearest evidence yet for quasiparticles in the normal state. Crucial aspects of the data such as the dispersion, superconducting gaps, and the bosonic coupling kink and associated weight transfer are robust to a possible breakdown of the sudden approximation., Comment: 15 pages, 3 figures

Using high-resolution angle-resolved photoemission spectroscopy on $Bi_{2}Sr_{2}CaCu_{2}O_{8+\delta}$, we have made the first observation of a mass renormalization or "kink" in the E vs. $\vec k$ dispersion relation localized near $(\pi, 0)$. Compared to the kink observed along the nodal direction, this new effect is clearly stronger, appears at a lower energy near 40 meV, and is only present in the superconducting state. The kink energy scale defines a cutoff below which well-defined quasiparticle excitations occur. This effect is likely due to coupling to a bosonic excitation, with the most plausible candidate being the magnetic resonance mode observed in inelastic neutron scattering.