J. J. Turner

Creation and diagnosis of a solid-density plasma with an X-ray free-electron laser

Matter with a high energy density (>105 joules per cm3) is prevalent throughout the Universe, being present in all types of stars and towards the centre of the giant planets; it is also relevant for inertial confinement fusion. Its thermodynamic and transport properties are challenging to measure, requiring the creation of sufficiently long-lived samples at homogeneous temperatures and densities. With the advent of the Linac Coherent Light Source (LCLS) X-ray laser, high-intensity radiation (>1017 watts per cm2, previously the domain of optical lasers) can be produced at X-ray wavelengths. The interaction of single atoms with such intense X-rays has recently been investigated. An understanding of the contrasting case of intense X-ray interaction with dense systems is important from a fundamental viewpoint and for applications. Here we report the experimental creation of a solid-density plasma at temperatures in excess of 106 kelvin on inertial-confinement timescales using an X-ray free-electron laser. We discuss the pertinent physics of the intense X-ray–matter interactions, and illustrate the importance of electron–ion collisions. Detailed simulations of the interaction process conducted with a radiative-collisional code show good qualitative agreement with the experimental results. We obtain insights into the evolution of the charge state distribution of the system, the electron density and temperature, and the timescales of collisional processes. Our results should inform future high-intensity X-ray experiments involving dense samples, such as X-ray diffractive imaging of biological systems, material science investigations, and the study of matter in extreme conditions.

Precision measurement of the weak mixing angle in Møller scattering

We report on a precision measurement of the parity-violating asymmetry in fixed target electron-electron (Møller) scattering: A(PV) = [-131 +/- 14(stat) +/- 10(syst)] x 10(-9), leading to the determination of the weak mixing angle sin2(thetaW(eff) = 0.2397 +/- 0.0010(stat) +/- 0.0008(syst), evaluated at Q2 = 0.026 GeV2. Combining this result with the measurements of sin2(thetaW(eff) at the Z0 pole, the running of the weak mixing angle is observed with over 6sigma significance. The measurement sets constraints on new physics effects at the TeV scale.

Nanoscale spin reversal by non-local angular momentum transfer following ultrafast laser excitation in ferrimagnetic GdFeCo

Ultrafast laser techniques have revealed extraordinary spin dynamics in magnetic materials that equilibrium descriptions of magnetism cannot explain. Particularly important for future applications is understanding non-equilibrium spin dynamics following laser excitation on the nanoscale, yet the limited spatial resolution of optical laser techniques has impeded such nanoscale studies. Here we present ultrafast diffraction experiments with an X-ray laser that probes the nanoscale spin dynamics following optical laser excitation in the ferrimagnetic alloy GdFeCo, which exhibits macroscopic all-optical switching. Our study reveals that GdFeCo displays nanoscale chemical and magnetic inhomogeneities that affect the spin dynamics. In particular, we observe Gd spin reversal in Gd-rich nanoregions within the first picosecond driven by the non-local transfer of angular momentum from larger adjacent Fe-rich nanoregions. These results suggest that a magnetic materials microstructure can be engineered to control transient laser-excited spins, potentially allowing faster (~ 1 ps) spin reversal than in present technologies.

Orbital-specific mapping of the ligand exchange dynamics of Fe(CO)(5) in solution

Transition-metal complexes have long attracted interest for fundamental chemical reactivity studies and possible use in solar energy conversion. Electronic excitation, ligand loss from the metal centre, or a combination of both, creates changes in charge and spin density at the metal site that need to be controlled to optimize complexes for photocatalytic hydrogen production and selective carbon–hydrogen bond activation. An understanding at the molecular level of how transition-metal complexes catalyse reactions, and in particular of the role of the short-lived and reactive intermediate states involved, will be critical for such optimization. However, suitable methods for detailed characterization of electronic excited states have been lacking. Here we show, with the use of X-ray laser-based femtosecond-resolution spectroscopy and advanced quantum chemical theory to probe the reaction dynamics of the benchmark transition-metal complex Fe(CO)5 in solution, that the photo-induced removal of CO generates the 16-electron Fe(CO)4 species, a homogeneous catalyst with an electron deficiency at the Fe centre, in a hitherto unreported excited singlet state that either converts to the triplet ground state or combines with a CO or solvent molecule to regenerate a penta-coordinated Fe species on a sub-picosecond timescale. This finding, which resolves the debate about the relative importance of different spin channels in the photochemistry of Fe(CO)5 (refs 4, 16,17,18,19 and 20), was made possible by the ability of femtosecond X-ray spectroscopy to probe frontier-orbital interactions with atom specificity. We expect the method to be broadly applicable in the chemical sciences, and to complement approaches that probe structural dynamics in ultrafast processes.

Large-Amplitude Spin Dynamics Driven by a THz Pulse in Resonance with an Electromagnon

Ultrafast Manipulation Multiferroic materials commonly show both magnetism and ferroelectricity, such that the electric field can be used to manipulate the magnetic order, and vice versa. Kubacka et al. (p. 1333, published online 6 March) used a strong terahertz electromagnetic pulse in resonance with an electromagnon—an excitation based on both electric and magnetic ordering—to control the spin dynamics of the multiferroic TbMnO3 on a sub-picosecond time scale and induce the rotation of the spin-cycloid plane of the material. The electric field of an electromagnetic pulse exerts ultrafast control on the spin dynamics of the multiferroic TbMnO3. Multiferroics have attracted strong interest for potential applications where electric fields control magnetic order. The ultimate speed of control via magnetoelectric coupling, however, remains largely unexplored. Here, we report an experiment in which we drove spin dynamics in multiferroic TbMnO3 with an intense few-cycle terahertz (THz) light pulse tuned to resonance with an electromagnon, an electric-dipole active spin excitation. We observed the resulting spin motion using time-resolved resonant soft x-ray diffraction. Our results show that it is possible to directly manipulate atomic-scale magnetic structures with the electric field of light on a sub-picosecond time scale.

Probing the transition state region in catalytic CO oxidation on Ru

Catching CO oxidation Details of the transition state that forms as carbon monoxide (CO) adsorbed on a ruthenium surface is oxidized to CO2 have been revealed by ultrafast excitation and probe methods. Öström et al. initiated the reaction between CO and adsorbed oxygen atoms with laser pulses that rapidly heated the surface and then probed the changes in electronic structure with oxygen x-ray absorption spectroscopy. They observed transition-state configurations that are consistent with density functional theory and a quantum oscillator model. Science, this issue p. 978 Ultrafast x-ray spectroscopy reveals electronic changes that occur during the oxidation of carbon monoxide on a ruthenium surface. Femtosecond x-ray laser pulses are used to probe the carbon monoxide (CO) oxidation reaction on ruthenium (Ru) initiated by an optical laser pulse. On a time scale of a few hundred femtoseconds, the optical laser pulse excites motions of CO and oxygen (O) on the surface, allowing the reactants to collide, and, with a transient close to a picosecond (ps), new electronic states appear in the O K-edge x-ray absorption spectrum. Density functional theory calculations indicate that these result from changes in the adsorption site and bond formation between CO and O with a distribution of OC–O bond lengths close to the transition state (TS). After 1 ps, 10% of the CO populate the TS region, which is consistent with predictions based on a quantum oscillator model.

The Stanford linear accelerator polarized electron source

The Stanford 3-km linear accelerator at SLAC has operated exclusively since early 1992 using a polarized electron beam for its high-energy physics programs. The polarized electron source now consists of a diode-type gun with a strained-lattice GaAs photocathode DC biased at high voltage and excited with circularly polarized photons generated by a pulsed, Ti:sapphire laser system. The electron polarization at the source is > 80%. To date the source has met all the beam requirements of the SLC and fixed target programs with < 5% downtime.

Few-femtosecond time-resolved measurements of X-ray free-electron lasers

X-ray free-electron lasers, with pulse durations ranging from a few to several hundred femtoseconds, are uniquely suited for studying atomic, molecular, chemical and biological systems. Characterizing the temporal profiles of these femtosecond X-ray pulses that vary from shot to shot is not only challenging but also important for data interpretation. Here we report the time-resolved measurements of X-ray free-electron lasers by using an X-band radiofrequency transverse deflector at the Linac Coherent Light Source. We demonstrate this method to be a simple, non-invasive technique with a large dynamic range for single-shot electron and X-ray temporal characterization. A resolution of less than 1 fs root mean square has been achieved for soft X-ray pulses. The lasing evolution along the undulator has been studied with the electron trapping being observed as the X-ray peak power approaches 100 GW.

Driving magnetic order in a manganite by ultrafast lattice excitation

Femtosecond midinfrared pulses are used to directly excite the lattice of the single-layer manganite La0.5Sr1.5MnO4. Magnetic and orbital orders, as measured by femtosecond resonant soft x-ray diffraction with an x-ray free-electron laser, are reduced within a few picoseconds. This effect is interpreted as a displacive exchange quench, a prompt shift in the equilibrium value of the magnetic- and orbital-order parameters after the lattice has been distorted. Control of magnetism through ultrafast lattice excitation may be of use for high-speed optomagnetism.

High-intensity double-pulse X-ray free-electron laser.

The X-ray free-electron laser has opened a new era for photon science, improving the X-ray brightness by ten orders of magnitude over previously available sources. Similar to an optical laser, the spectral and temporal structure of the radiation pulses can be tailored to the specific needs of many experiments by accurately manipulating the lasing medium, that is, the electron beam. Here we report the generation of mJ-level two-colour hard X-ray pulses of few femtoseconds duration with an XFEL driven by twin electron bunches at the Linac Coherent Light Source. This performance represents an improvement of over an order of magnitude in peak power over state-of-the-art two-colour XFELs. The unprecedented intensity and temporal coherence of this new two-colour X-ray free-electron laser enable an entirely new set of scientific applications, ranging from X-ray pump/X-ray probe experiments to the imaging of complex biological samples with multiple wavelength anomalous dispersion.