Resonant Inelastic X-Ray Scattering Reveals Hidden Local Transitions of the Aqueous OH Radical.

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.

Nonlinear Ultrafast Spin Scattering in the Skyrmion Phase of Cu_{2}OSeO_{3}.

Ultrafast x-ray scattering studies of the topological Skyrmion phase in Cu_{2}OSeO_{3} show the dynamics to be strongly dependent on the excitation energy and fluence. At high photon energies, where the electron-spin scattering cross section is relatively high, the excitation of the topological Skyrmion phase shows a nonlinear dependence on the excitation fluence, in contrast to the excitation of the conical phase which is linearly dependent on the excitation fluence. The excitation of the Skyrmion order parameter is nonlinear in the magnetic excitation resulting from scattering during electron-hole recombination, indicating different dominant scattering processes in the conical and Skyrmion phases.

Nanosecond X-Ray Photon Correlation Spectroscopy on Magnetic Skyrmions.

We report an x-ray photon correlation spectroscopy method that exploits the recent development of the two-pulse mode at the Linac Coherent Light Source. By using coherent resonant x-ray magnetic scattering, we studied spontaneous fluctuations on nanosecond time scales in thin films of multilayered Fe/Gd that exhibit ordered stripe and Skyrmion lattice phases. The correlation time of the fluctuations was found to differ between the Skyrmion phase and near the stripe-Skyrmion boundary. This technique will enable a significant new area of research on the study of equilibrium fluctuations in condensed matter.

Emergence of the persistent spin helix in semiconductor quantum wells.

According to Noether's theorem, for every symmetry in nature there is a corresponding conservation law. For example, invariance with respect to spatial translation corresponds to conservation of momentum. In another well-known example, invariance with respect to rotation of the electron's spin, or SU(2) symmetry, leads to conservation of spin polarization. For electrons in a solid, this symmetry is ordinarily broken by spin-orbit coupling, allowing spin angular momentum to flow to orbital angular momentum. However, it has recently been predicted that SU(2) can be achieved in a two-dimensional electron gas, despite the presence of spin-orbit coupling. The corresponding conserved quantities include the amplitude and phase of a helical spin density wave termed the 'persistent spin helix'. SU(2) is realized, in principle, when the strengths of two dominant spin-orbit interactions, the Rashba (strength parameterized by alpha) and linear Dresselhaus (beta(1)) interactions, are equal. This symmetry is predicted to be robust against all forms of spin-independent scattering, including electron-electron interactions, but is broken by the cubic Dresselhaus term (beta(3)) and spin-dependent scattering. When these terms are negligible, the distance over which spin information can propagate is predicted to diverge as alpha approaches beta(1). Here we report experimental observation of the emergence of the persistent spin helix in GaAs quantum wells by independently tuning alpha and beta(1). Using transient spin-grating spectroscopy, we find a spin-lifetime enhancement of two orders of magnitude near the symmetry point. Excellent quantitative agreement with theory across a wide range of sample parameters allows us to obtain an absolute measure of all relevant spin-orbit terms, identifying beta(3) as the main SU(2)-violating term in our samples. The tunable suppression of spin relaxation demonstrated in this work is well suited for application to spintronics.

Attosecond-pump attosecond-probe x-ray spectroscopy of liquid water.

Attosecond-pump/attosecond-probe experiments have long been sought as the most straightforward method for observing electron dynamics in real time. Although there has been much success with overlapped near-infrared femtosecond and extreme ultraviolet attosecond pulses combined with theory, true attosecond-pump/attosecond-probe experiments have been limited. We used a synchronized attosecond x-ray pulse pair from an x-ray free-electron laser to study the electronic response to valence ionization in liquid water through all x-ray attosecond transient absorption spectroscopy (AX-ATAS). Our analysis showed that the AX-ATAS response is confined to the subfemtosecond timescale, eliminating any hydrogen atom motion and demonstrating experimentally that the 1b1 splitting in the x-ray emission spectrum is related to dynamics and is not evidence of two structural motifs in ambient liquid water.

Time-resolved optical reflectivity of the electron-doped Nd(2-x)Ce(x)CuO(4+δ) cuprate superconductor: evidence for an interplay between competing orders.

We use pump-probe spectroscopy to measure the photoinduced reflectivity ΔR of the electron-doped cuprate superconductor Nd(2-x)Ce(x)CuO(4+δ) at a value of x near optimal doping, as a function of time, temperature, and laser fluence. We observe the onset of a negative ΔR signal at T(*)≈75 K, above the superconducting transition temperature, T(c), of 23 K. The relatively slow decay of ΔR, compared to the analogous signal in hole doped compounds, allows us to resolve time-temperature scaling consistent with critical fluctuations. A positive ΔR signal 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 another fluctuating order.

Coherent propagation of spin helices in a quantum-well confined electron gas.

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).

Observation of coherent helimagnons and gilbert damping in an itinerant magnet.

We study the magnetic excitations of itinerant helimagnets by applying time-resolved optical spectroscopy to Fe(0.8)Co(0.2)Si. 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.

Enhanced charge density wave coherence in a light-quenched, high-temperature superconductor.

Superconductivity and charge density waves (CDWs) 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 scale is necessary. We use ultrafast resonant soft x-ray scattering to track the transient evolution of CDW correlations in YBa2Cu3O6+x after the quench of superconductivity by an infrared laser pulse. We observe a nonthermal response of the CDW order characterized by a near doubling of the correlation length within ≈1 picosecond of the superconducting quench. Our results are consistent with a model in which the interaction between superconductivity and CDWs manifests inhomogeneously through disruption of spatial coherence, with superconductivity playing the dominant role in stabilizing CDW topological defects, such as discommensurations.

Measurement of electron-hole friction in an n-doped GaAs/AlGaAs quantum well using optical transient grating spectroscopy.

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.

Low-energy (<10 meV) feature in the nodal electron self-energy and strong temperature dependence of the Fermi velocity in Bi{2}Sr{2}CaCu{2}O{8+δ}.

Using low photon energy angle-resolved photoemission, we study the low-energy dispersion along the nodal (π,π) direction in Bi{2}Sr{2}CaCu{2}O{8+δ} as a function of temperature. Less than 10 meV below the Fermi energy, the high-resolution data reveal a novel "kinklike" feature in 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 at higher temperatures. A corollary of this finding is that the Fermi velocity v{F}, as measured in this low-energy range, varies rapidly with temperature-increasing by almost 30% from 70 to 110 K. The behavior of v{F}(T) appears to shift as a function of doping, suggesting a departure from simple "universality" in the nodal Fermi velocity of cuprates.

Experimental setup for low-energy laser-based angle resolved photoemission spectroscopy.

A laser-based angle resolved photoemission (ARPES) 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 Bi(2)Sr(2)CaCu(2)O(8+delta) (Bi2212) is compared to the results from higher photon energies.

The rate of quasiparticle recombination probes the onset of coherence in cuprate superconductors.

In the underdoped copper-oxides, high-temperature superconductivity condenses 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. This CDW coexists and competes with superconductivity (SC) below the transition temperature Tc, suggesting that these two orders 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, τqp, as a function of temperature and magnetic field in underdoped HgBa2CuO(4+δ) (Hg-1201) and YBa2Cu3O(6+x) (YBCO) single crystals by ultrafast time-resolved reflectivity. We find that τqp(T) exhibits a local maximum in a small temperature window near Tc 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 Tc 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.

From a single-band metal to a high-temperature superconductor via two thermal phase transitions.

The nature of the pseudogap phase of cuprate high-temperature superconductors is a major unsolved problem in condensed matter physics. We studied the commencement of the pseudogap state at temperature T* using three different techniques (angle-resolved photoemission spectroscopy, polar Kerr effect, and time-resolved reflectivity) on the same optimally doped Bi2201 crystals. We observed the coincident, abrupt onset at T* of a particle-hole asymmetric antinodal gap in the electronic spectrum, a Kerr rotation in the reflected light polarization, and a change in the ultrafast relaxational dynamics, consistent with a phase transition. Upon further cooling, spectroscopic signatures of superconductivity begin to grow close to the superconducting transition temperature (T(c)), entangled in an energy-momentum-dependent manner with the preexisting pseudogap features, ushering in a ground state with coexisting orders.

Laser based angle-resolved photoemission, the sudden approximation, and quasiparticle-like spectral peaks in Bi2Sr2CaCu2O(8+delta).

A new low photon energy regime of angle-resolved photoemission spectroscopy is accessed with lasers and used to study the high T(C) superconductor Bi2Sr2CaCu2O(8+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 are found to be robust to a possible breakdown of the sudden approximation.