Soft X-ray seeding studies for the SLAC Linac Coherent Light Source II

We present the results from studies of soft X-ray seeding options for the LCLS-II X-ray free electron laser (FEL) at SLAC. The LCLS-II will use superconducting accelerator technology to produce X-ray pulses at up to 1 MHz repetition rate using 4 GeV electron beams. If properly seeded, these pulses will be nearly fully coherent, and highly stable in photon energy, bandwidth, and intensity, thus enabling unique experiments with intense high-resolution soft X-rays. Given the expected electron beam parameters from start to end simulations and predicted FEL performance, our studies reveal echo enabled harmonic generation (EEHG) and soft X-ray self-seeding (SXRSS) as promising and complementary seeding methods. We find that SXRSS has the advantage of simplicity and will deliver 5-35 times higher spectral brightness than EEHG in the 1-2 nm range, but lacks some of the potential for phase-stable multipulse and multicolor FEL operations enabled by external laser seeding with EEHG

Ultrafast Laser-Induced Melting of Long-Range Magnetic Order in Multiferroic TbMnO3

We performed ultrafast time-resolved near-infrared pump, resonant soft X-ray diffraction probe measurements to investigate the coupling between the photoexcited electronic system and the spin cycloid magnetic order in multiferroic TbMnO3 at low temperatures. We observe melting of the long range antiferromagnetic order at low excitation fluences with a decay time constant of 22.3 +- 1.1 ps, which is much slower than the ~1 ps melting times previously observed in other systems. To explain the data we propose a simple model of the melting process where the pump laser pulse directly excites the electronic system, which then leads to an increase in the effective temperature of the spin system via a slower relaxation mechanism. Despite this apparent increase in the effective spin temperature, we do not observe changes in the wavevector q of the antiferromagnetic spin order that would typically correlate with an increase in temperature under equilibrium conditions. We suggest that this behavior results from the extremely low magnon group velocity that hinders a change in the spin-spiral wavevector on these time scales.Comment: 9 pages, 4 figure

Optically induced lattice deformations, electronic structure changes, and enhanced superconductivity in YBa2Cu3O6.48

Resonant optical excitation of apical oxygen vibrational modes in the normal state of underdoped YBa2Cu3O6+x induces a transient state with optical properties similar to those of the equilibrium superconducting state. Amongst these, a divergent imaginary conductivity and a plasma edge are transiently observed in the photo-stimulated state. Femtosecond hard x-ray diffraction experiments have been used in the past to identify the transient crystal structure in this non-equilibrium state. Here, we start from these crystallographic features and theoretically predict the corresponding electronic rearrangements that accompany these structural deformations. Using density functional theory, we predict enhanced hole-doping of the CuO2 planes. The empty chain Cu dy2-z2 orbital is calculated to strongly reduce in energy, which would increase c-axis transport and potentially enhance the interlayer Josephson coupling as observed in the THz-frequency response. From these calculations, we predict changes in the soft x-ray absorption spectra at the Cu L-edge. Femtosecond x-ray pulses from a free electron laser are used to probe these changes in absorption at two photon energies along this spectrum, and provide data consistent with these predictions.Comment: 20 pages with 6 figure

Probing the interplay between lattice dynamics and short-range magnetic correlations in CuGeO3 with femtosecond RIXS

Investigations of magnetically ordered phases on the femtosecond timescale have provided significant insights into the influence of charge and lattice degrees of freedom on the magnetic sub-system. However, short-range magnetic correlations occurring in the absence of long-range order, for example in spin-frustrated systems, are inaccessible to many ultrafast techniques. Here, we show how time-resolved resonant inelastic X-ray scattering (trRIXS) is capable of probing such short-ranged magnetic dynamics in a charge-transfer insulator through the detection of a Zhang-Rice singlet exciton. Utilizing trRIXS measurements at the O K-edge, and in combination with model calculations, we probe the short-range spin-correlations in the frustrated spin chain material CuGeO3 following photo-excitation, revealing a strong coupling between the local lattice and spin sub-systems

Strong Influence of Coadsorbate Interaction on CO Desorption Dynamics on Ru(0001) Probed by Ultrafast X-Ray Spectroscopy and \u3cem\u3eAb Initio\u3c/em\u3e Simulations

We show that coadsorbed oxygen atoms have a dramatic influence on the CO desorption dynamics from Ru(0001). In contrast to the precursor-mediated desorption mechanism on Ru(0001), the presence of surface oxygen modifies the electronic structure of Ru atoms such that CO desorption occurs predominantly via the direct pathway. This phenomenon is directly observed in an ultrafast pump-probe experiment using a soft x-ray free-electron laser to monitor the dynamic evolution of the valence electronic structure of the surface species. This is supported with the potential of mean force along the CO desorption path obtained from density-functional theory calculations. Charge density distribution and frozen-orbital analysis suggest that the oxygen-induced reduction of the Pauli repulsion, and consequent increase of the dative interaction between the CO 5σ and the charged Ru atom, is the electronic origin of the distinct desorption dynamics. Ab initio molecular dynamics simulations of CO desorption from Ru(0001) and oxygen-coadsorbed Ru(0001) provide further insights into the surface bond-breaking process

X ray emission spectroscopy of bulk liquid water in no man s land

The structure of bulk liquid water was recently probed by x ray scattering below the temperature limit of homogeneous nucleation TH of amp; 8764;232 K [J. A. Sellberg et al., Nature 510, 381 384 2014 ]. Here, we utilize a similar approach to study the structure of bulk liquid water below TH using oxygen K edge x ray emission spectroscopy XES . Based on previous XES experiments [T. Tokushima et al., Chem. Phys. Lett. 460, 387 400 2008 ] at higher temperatures, we expected the ratio of the 1b1 amp; 8242; and 1b1 amp; 8242; amp; 8242; peaks associated with the lone pair orbital in water to change strongly upon deep supercooling as the coordination of the hydrogen H bonds becomes tetrahedral. In contrast, we observed only minor changes in the lone pair spectral region, challenging an interpretation in terms of two interconverting species. A number of alternative hypotheses to explain the results are put forward and discussed. Although the spectra can be explained by various contributions from these hypotheses, we here emphasize the interpretation that the line shape of each component changes dramatically when approaching lower temperatures, where, in particular, the peak assigned to the proposed disordered component would become more symmetrical as vibrational interference becomes more importan