Erratum: Delayed Onset of Nonthermal Melting in Single-Crystal Silicon Pumped with Hard X Rays [Phys. Rev. Lett. 120, 265701 (2018)].

This corrects the article DOI: 10.1103/PhysRevLett.120.265701.

Delayed Onset of Nonthermal Melting in Single-Crystal Silicon Pumped with Hard X Rays.

In this work, we monitor the onset of nonthermal melting in single-crystal silicon by implementing an x-ray pump-x-ray probe scheme. Using the ultrashort pulses provided by the Linac Coherent Light Source (SLAC) and a custom-built split-and-delay line for hard x rays, we achieve the temporal resolution needed to detect the onset of the transition. Our data show no loss of long-range order up to 150±40 fs from photoabsorption, which we interpret as the time needed for the electronic system to equilibrate at or above the critical nonthermal melting temperature. Once such equilibration is reached, the loss of long-range atomic order proceeds inertially and is completed within 315±40 fs from photoabsorption.

Characterization and simulation of soft gamma-ray mirrors for their use with spent fuel rods at reprocessing facilities.

The use of a grazing incidence optic to selectively reflect K-shell fluorescence emission and isotope-specific lines from special nuclear materials is a highly desirable nondestructive analysis method for use in reprocessing fuel environments. Preliminary measurements have been performed, and a simulation suite has been developed to give insight into the design of the x ray optics system as a function of the source emission, multilayer coating characteristics, and general experimental configurations. The experimental results are compared to the predictions from our simulation toolkit to illustrate the ray-tracing capability and explore the effect of modified optics in future measurement campaigns.

Absolute pulse energy measurements of soft x-rays at the Linac Coherent Light Source.

This paper reports novel measurements of x-ray optical radiation on an absolute scale from the intense and ultra-short radiation generated in the soft x-ray regime of a free electron laser. We give a brief description of the detection principle for radiation measurements which was specifically adapted for this photon energy range. We present data characterizing the soft x-ray instrument at the Linac Coherent Light Source (LCLS) with respect to the radiant power output and transmission by using an absolute detector temporarily placed at the downstream end of the instrument. This provides an estimation of the reflectivity of all x-ray optical elements in the beamline and provides the absolute photon number per bandwidth per pulse. This parameter is important for many experiments that need to understand the trade-offs between high energy resolution and high flux, such as experiments focused on studying materials via resonant processes. Furthermore, the results are compared with the LCLS diagnostic gas detectors to test the limits of linearity, and observations are reported on radiation contamination from spontaneous undulator radiation and higher harmonic content.

Temporal cross-correlation of x-ray free electron and optical lasers using soft x-ray pulse induced transient reflectivity.

The recent development of x-ray free electron lasers providing coherent, femtosecond-long pulses of high brilliance and variable energy opens new areas of scientific research in a variety of disciplines such as physics, chemistry, and biology. Pump-probe experimental techniques which observe the temporal evolution of systems after optical or x-ray pulse excitation are one of the main experimental schemes currently in use for ultrafast studies. The key challenge in these experiments is to reliably achieve temporal and spatial overlap of the x-ray and optical pulses. Here we present measurements of the x-ray pulse induced transient change of optical reflectivity from a variety of materials covering the soft x-ray photon energy range from 500eV to 2000eV and outline the use of this technique to establish and characterize temporal synchronization of the optical-laser and FEL x-ray pulses.

Coherence properties of individual femtosecond pulses of an x-ray free-electron laser.

Measurements of the spatial and temporal coherence of single, femtosecond x-ray pulses generated by the first hard x-ray free-electron laser, the Linac Coherent Light Source, are presented. Single-shot measurements were performed at 780 eV x-ray photon energy using apertures containing double pinholes in "diffract-and-destroy" mode. We determined a coherence length of 17 µm in the vertical direction, which is approximately the size of the focused Linac Coherent Light Source beam in the same direction. The analysis of the diffraction patterns produced by the pinholes with the largest separation yields an estimate of the temporal coherence time of 0.55 fs. We find that the total degree of transverse coherence is 56% and that the x-ray pulses are adequately described by two transverse coherent modes in each direction. This leads us to the conclusion that 78% of the total power is contained in the dominant mode.

Ultrafast multi-cycle terahertz measurements of the electrical conductivity in strongly excited solids.

Key insights in materials at extreme temperatures and pressures can be gained by accurate measurements that determine the electrical conductivity. Free-electron laser pulses can ionize and excite matter out of equilibrium on femtosecond time scales, modifying the electronic and ionic structures and enhancing electronic scattering properties. The transient evolution of the conductivity manifests the energy coupling from high temperature electrons to low temperature ions. Here we combine accelerator-based, high-brightness multi-cycle terahertz radiation with a single-shot electro-optic sampling technique to probe the evolution of DC electrical conductivity using terahertz transmission measurements on sub-picosecond time scales with a multi-undulator free electron laser. Our results allow the direct determination of the electron-electron and electron-ion scattering frequencies that are the major contributors of the electrical resistivity.

Interaction of short x-ray pulses with low-Z x-ray optics materials at the LCLS free-electron laser.

Materials used for hard x-ray-free-electron laser (XFEL) optics must withstand high-intensity x-ray pulses. The advent of the Linac Coherent Light Source has enabled us to expose candidate optical materials, such as bulk B4C and SiC films, to 0.83 keV XFEL pulses with pulse energies between 1 µJ and 2 mJ to determine short-pulse hard x-ray damage thresholds. The fluence required for the onset of damage for single pulses is around the melt fluence and slightly lower for multiple pulses. We observed strong mechanical cracking in the materials, which may be due to the larger penetration depths of the hard x-rays.

A new streaked soft x-ray imager for the National Ignition Facility.

A new streaked soft x-ray imager has been designed for use on high energy-density (HED) physics experiments at the National Ignition Facility based at the Lawrence Livermore National Laboratory. This streaked imager uses a slit aperture, single shallow angle reflection from a nickel mirror, and soft x-ray filtering to, when coupled to one of the NIF's x-ray streak cameras, record a 4× magnification, one-dimensional image of an x-ray source with a spatial resolution of less than 90 µm. The energy band pass produced depends upon the filter material used; for the first qualification shots, vanadium and silver-on-titanium filters were used to gate on photon energy ranges of approximately 300-510 eV and 200-400 eV, respectively. A two-channel version of the snout is available for x-ray sources up to 1 mm and a single-channel is available for larger sources up to 3 mm. Both the one and two-channel variants have been qualified on quartz wire and HED physics target shots.

Two-color spatial and temporal temperature measurements using a streaked soft x-ray imager.

A dual-channel streaked soft x-ray imager has been designed and used on high energy-density physics experiments at the National Ignition Facility. This streaked imager creates two images of the same x-ray source using two slit apertures and a single shallow angle reflection from a nickel mirror. Thin filters are used to create narrow band pass images at 510 eV and 360 eV. When measuring a Planckian spectrum, the brightness ratio of the two images can be translated into a color-temperature, provided that the spectral sensitivity of the two images is well known. To reduce uncertainty and remove spectral features in the streak camera photocathode from this photon energy range, a thin 100 nm CsI on 50 nm Al streak camera photocathode was implemented. Provided that the spectral shape is well-known, then uncertainties on the spectral sensitivity limits the accuracy of the temperature measurement to approximately 4.5% at 100 eV.

Reflective multilayer optic as hard X-ray diagnostic on laser-plasma experiment.

A multilayer-based optic was tested for use as an X-ray diagnostic on a laser-plasma experiment. The multilayer optic was employed to selectively pass X-rays between 55 and 100 keV. An order of magnitude improvement in signal-to-noise ratio is achieved compared to a transmission crystal spectrometer. A multilayer response model, taking into account the source size and spectral content, is constructed and the outlook for application above 500 keV is briefly discussed. LLNL-JRNL-664311.

The soft x-ray instrument for materials studies at the linac coherent light source x-ray free-electron laser.

The soft x-ray materials science instrument is the second operational beamline at the linac coherent light source x-ray free electron laser. The instrument operates with a photon energy range of 480-2000 eV and features a grating monochromator as well as bendable refocusing mirrors. A broad range of experimental stations may be installed to study diverse scientific topics such as: ultrafast chemistry, surface science, highly correlated electron systems, matter under extreme conditions, and laboratory astrophysics. Preliminary commissioning results are presented including the first soft x-ray single-shot energy spectrum from a free electron laser.

Soft x-ray images of the laser entrance hole of ignition hohlraums.

Hohlraums are employed at the national ignition facility to convert laser energy into a thermal x-radiation drive, which implodes a fusion capsule, thus compressing the fuel. The x-radiation drive is measured with a low spectral resolution, time-resolved x-ray spectrometer, which views the region around the hohlraum's laser entrance hole. This measurement has no spatial resolution. To convert this to the drive inside the hohlraum, the size of the hohlraum's opening ("clear aperture") and fraction of the measured x-radiation, which comes from this opening, must be known. The size of the clear aperture is measured with the time integrated static x-ray imager (SXI). A soft x-ray imaging channel has been added to the SXI to measure the fraction of x-radiation emitted from inside the clear aperture. A multilayer mirror plus filter selects an x-ray band centered at 870 eV, near the peak of the x-ray spectrum of a 300 eV blackbody. Results from this channel and corrections to the x-radiation drive are discussed.

Pulse-dilation enhanced gated optical imager with 5 ps resolution (invited).

A 5 ps gated framing camera was demonstrated using the pulse-dilation of a drifting electron signal. The pulse-dilation is achieved by accelerating a photoelectron derived information pulse with a time varying potential [R. D. Prosser, J. Phys. E 9, 57 (1976)]. The temporal dependence of the accelerating potential causes a birth time dependent axial velocity dispersion that spreads the pulse as it transits a drift region. The expanded pulse is then imaged with a conventional gated microchannel plate based framing camera and the effective gating time of the combined instrument is reduced over that of the framing camera alone. In the drift region, electron image defocusing in the transverse or image plane is prevented with a large axial magnetic field. Details of the unique issues associated with rf excited photocathodes were investigated numerically and a prototype instrument based on this principle was recently constructed. Temporal resolution of the instrument was measured with a frequency tripled femtosecond laser operating at 266 nm. The system demonstrated 20× temporal magnification and the results are presented here. X-ray image formation strategies and photometric calculations for inertial confinement fusion implosion experiments are also examined.

Reflectance measurements on clean surfaces for the determination of optical constants of silicon in the extreme ultraviolet-soft-x-ray region.

The refractive index n = 1 - delta + ibeta of Si in the energy range 50-180 eV is investigated with angle-dependent reflectance measurements. The optical constants delta and beta are both determined by fitting to the Fresnel equations. The results of this method are compared with the values in the atomic tables derived from experimental data for beta and implementation of the Kramers-Kronig relations for delta. The samples were prepared by UV irradiation and HF:ethanol dipping to H passivate the surface. It is found that the values of delta in the atomic tables are 8-15% too high in the region 50-90 eV. This is attributed to missing oscillator strength in the tabulated absorption coefficient for Si. The measured values of beta for crystalline Si exhibit structure below the L (2,3) edge (99.8 eV), as was previously observed in transmission measurements of Si(111). It is also found that the method of least-squares fitting reflectance data to obtain optical constants is most effective for energies well below the edge, where delta > beta, while for a range of energies around and above the edge, where delta < beta, the optical constants are determined with large uncertainties. This behavior is not unique to the Si L(2,3) edge.

Absolute Photoabsorption Measurements of Molybdenum in the Range 60-930 eV for Optical Constant Determination.

Transmission measurements for the optical constants delta, beta of thecomplex refractive index n = 1 - delta + ibeta of molybdenum are performed in the energy range 60-930eV. Free-standing C/Mo/C foils of five different thicknesses are used, and the results are normalized for the presence of the carbon layers in the samples. These absorption results are combined with previous experimental data in the lower energy range and values fromthe atomic tables to obtain the imaginary (absorptive) part of the refractive index for molybdenum in the range 1-30,000 eV. The real(dispersive) part of n was calculated from Kramers-Kronig analysis with the above absorption data. An evaluation with the partial sum rules demonstrates that this new compilation provides an improved set of values for n covering a wider energy range compared with the current tabulated values. The new results are applied so as to calculate thenormal-incidence reflectivities of Mo/Si and Mo/Be multilayer mirrors.

Molybdenum/beryllium multilayer mirrors for normal incidence in the extreme ultraviolet.

We report on a series of normal-incidence reflectance measurements at wavelengths just longer than the beryllium K-edge (11.1 nm) from molybdenum/beryllium multilayer mirrors. The highest peak reflectance was 68.7 ± 0.2% at λ = 11.3 nm obtained from a mirror with 70 bilayers ending in beryllium. To our knowledge, this is the highest normal-incidence reflectance that has been demonstrated in the 1-80-nm spectral range.