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Electromagnetic and electrostatic levitation techniques have been utilized for the last few decades to process metastable and highly reactive materials. Main fields of application include thermophysical properties, solidification, and transport phenomena of molten metals, which are of critical importance to better understand and control manufacturing processes dealing with molten metals, such as casting, welding, and additive manufacturing. This paper addresses part of our international collaborative work with NASA, European Space Agency, German Aerospace Center, and Japanese Aerospace Exploration Agency to support containerless experiments aboard the International Space Station. Along with space experiments, our recent work using an electrostatic levitator to unveil the liquid structure of aqueous sodium sulfate solutions (the most damaging salt to civil structures) is also introduced.

We characterize the spatial and temporal coherence properties of hard X-ray pulses from the Pohang Accelerator Laboratory X-ray Free Electron Laser (PAL-XFEL, Pohang, Korea). The measurement of the single-shot speckle contrast, together with the introduction of corrections considering experimental conditions, allows obtaining an intrinsic degree of transverse coherence of 0.85 ± 0.06. In the Self-Amplified Spontaneous Emission regime, the analysis of the intensity distribution of X-ray pulses also provides an estimate for the number of longitudinal modes. For monochromatic and pink (i.e. natural bandwidth provided by the first harmonic of the undulator) beams, we observe that the number of temporal modes is 6.0 ± 0.4 and 90.0 ± 7.2, respectively. Assuming a coherence time of 2.06 fs and 0.14 fs for the monochromatic and pink beam respectively, we estimate an average X-ray pulse duration of 12.6 ± 1.0 fs.

New journal of physics 20(3), 033008 (2018). doi:10.1088/1367-2630/aab548, Arbitrary manipulation of the temporal and spectral properties of x-ray pulses at free-electron lasers would revolutionize many experimental applications. At the Linac Coherent Light Source at Stanford National Accelerator Laboratory, the momentum phase-space of the free-electron laser driving electron bunch can be tuned to emit a pair of x-ray pulses with independently variable photon energy and femtosecond delay. However, while accelerator parameters can easily be adjusted to tune the electron bunch phase-space, the final impact of these actuators on the x-ray pulse cannot be predicted with sufficient precision. Furthermore, shot-to-shot instabilities that distort the pulse shape unpredictably cannot be fully suppressed. Therefore, the ability to directly characterize the x-rays is essential to ensure precise and consistent control. In this work, we have generated x-ray pulse pairs via electron bunch shaping and characterized them on a single-shot basis with femtosecond resolution through time-resolved photoelectron streaking spectroscopy. This achievement completes an important step toward future x-ray pulse shaping techniques., Published by IOP, [London]

A description of the X-ray Correlation Spectroscopy instrument at the Linac Coherent Light Source is presented. Recent highlights illustrate the coherence properties of the source as well as some recent dynamics measurements and future directions., The X-ray Correlation Spectroscopy instrument is dedicated to the study of dynamics in condensed matter systems using the unique coherence properties of free-electron lasers. It covers a photon energy range of 4–25 keV. The intrinsic temporal characteristics of the Linac Coherent Light Source, in particular the 120 Hz repetition rate, allow for the investigation of slow dynamics (milli­seconds) by means of X-ray photon correlation spectroscopy. Double-pulse schemes could probe dynamics on the picosecond timescale. A description of the instrument capabilities and recent achievements is presented.

Nonlinear optical phenomena in semiconductors present several fundamental problems in modern optics that are of great importance for the development of optoelectronic devices. In particular, the details of photo-induced lattice dynamics at early time-scales prior to carrier recombination remain poorly understood. We demonstrate the first integrated measurements of both optical and structural, material-dependent quantities while also inferring the bulk impulsive strain profile by using high spatial-resolution time-resolved x-ray scattering (TRXS) on bulk crystalline gallium arsenide. Our findings reveal distinctive laser-fluence dependent crystal lattice responses, which are not described by previous TRXS experiments or models. The initial linear expansion of the crystal upon laser excitation stagnates at a laser fluence corresponding to the saturation of the free carrier density before resuming expansion in a third regime at higher fluences where two-photon absorption becomes dominant. Our interpretations of the lattice dynamics as nonlinear optical effects are confirmed by numerical simulations and by additional measurements in an n-type semiconductor that allows higher-order nonlinear optical processes to be directly observed as modulations of x-ray diffraction lineshapes.

In this paper we describe a setup for x-ray scattering experiments on complex fluids using a liquid jet. The setup supports Small and Wide Angle X-ray Scattering (SAXS/WAXS) geometries. The jet is formed by a gas-dynamic virtual nozzle (GDVN) allowing for diameters ranging between 1 μm and 20 μm at a jet length of several hundred μm. To control jet properties such as jet length, diameter, or flow rate, the instrument is equipped with several diagnostic tools. Three microscopes are installed to quantify jet dimensions and stability in situ. The setup has been used at several beamlines performing both SAXS and WAXS experiments. As a typical example we show an experiment on a colloidal dispersion in a liquid jet at the X-ray Correlation Spectroscopy instrument at the Linac Coherent Light Source free-electron laser.

We show that time-resolved x-ray scattering can be applied to polycrystalline materials for the measurement of carrier diffusion. A polycrystalline indium antimonide sample is prepared by high-intensity ultrafast laser surface melting and re-solidification under vacuum to create randomly oriented grains with an average size of 13 nm. Two static diffraction rings are simultaneously observed on a gated pixel array detector. Their centroids move following lower-intensity laser excitation, and utilizing an in-situ angular calibration, the transient lattice spacing is determined with femtometer accuracy, thereby allowing the measurement of charge carrier dynamics. Compared to bulk calculations, we find that carrier diffusion slows by more than one order of magnitude. This result provides evidence for the formation of potential energy barriers at the grain boundaries and demonstrates the capability of time-resolved x-ray scattering to probe nanoscale charge transport in materials other than near-perfect crystals.We show that time-resolved x-ray scattering can be applied to polycrystalline materials for the measurement of carrier diffusion. A polycrystalline indium antimonide sample is prepared by high-intensity ultrafast laser surface melting and re-solidification under vacuum to create randomly oriented grains with an average size of 13 nm. Two static diffraction rings are simultaneously observed on a gated pixel array detector. Their centroids move following lower-intensity laser excitation, and utilizing an in-situ angular calibration, the transient lattice spacing is determined with femtometer accuracy, thereby allowing the measurement of charge carrier dynamics. Compared to bulk calculations, we find that carrier diffusion slows by more than one order of magnitude. This result provides evidence for the formation of potential energy barriers at the grain boundaries and demonstrates the capability of time-resolved x-ray scattering to probe nanoscale charge transport in materials other than near-perfect crystals.

We report on the development of a new experimental instrument for time-resolved x-ray scattering (TRXS) at the Pohang Light Source (PLS-II). It operates with a photon energy ranging from 5 to 18 keV. It is equipped with an amplified Ti:sappahire femtosecond laser, optical diagnostics, and laser beam delivery for pump-probe experiments. A high-speed single-element detector and high trigger-rate oscilloscope are used for rapid data acquisition. While this instrument is capable of measuring sub-nanosecond dynamics using standard laser pump/x-ray probe techniques, it also takes advantage of the dense 500 MHz standard fill pattern in the PLS-II storage ring to efficiently record nano-to-micro-second dynamics simultaneously. We demonstrate this capability by measuring both the (fast) impulsive strain and (slower) thermal recovery dynamics of a crystalline InSb sample following intense ultrafast laser excitation. Exploiting the full repetition rate of the storage ring results in a significant improvement in data collection rates compared to conventional bunch-tagging methods.

A hard X-ray delay line device capable of splitting single FEL X-ray pulses into two adjustable fractions and recombining them with the goal of performing X-ray Photon Correlation Spectroscopy and pump - probe type studies was designed. The performance of the device has been verified at the XPP and XCS instruments of LCLS. The measured throughput of the device at 7.9 keV is 3.6%. The coherence properties of the LCLS beam passing through the delay line were investigated by analyzing speckle patterns produced by single LCLS pulses. A high speckle contrast of 0.69 was found, indicating the feasibility of performing coherence based experiments with the delay line.

Physical review letters 109, 185502 (2012). doi:10.1103/PhysRevLett.109.185502, Published by APS, College Park, Md.

We report on the feasibility of high wavevector temporal speckle correlation measurements at the world’s first hard x-ray free electron laser, the Linac Coherent Light Source (LCLS). Due to the chaotic nature of LCLS, the spectral profile of the x-ray radiation fluctuates on a pulse-to-pulse basis. Its impact on the determination of the single shot speckle contrast in a wide angle x-ray scattering geometry is investigated by analyzing FEL power spectra that are simulated based on the nominal operational parameters of LCLS. Ultimately, a potential scheme to deliver a single-mode hard x-ray pulse is proposed by using a narrow bandpass crystal monochromator.

This content may be downloaded for personal use only. Any other use requires prior permission of the author and AIP Publishing. This material originally appeared in Review of Scientific Instruments 83, 043107 (2012) and may be found at https://doi.org/10.1063/1.3698294., 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.

An inline diagnostics device was developed to measure the intrinsic shot-to-shot intensity and position fluctuations of the SASE-based LCLS hard X-ray FEL source. The device is based on the detection of back-scattered X-rays from a partially-transmissive thin target using a quadrant X-ray diode array. This intensity and position monitor was tested for the first time with FEL X-rays on the XPP instrument of the LCLS. Performance analyses showed that the relative precision for intensity measurements approached 0.1% and the position sensitivity was better than 5 μm, limited only by the Poisson statistics of the X-rays collected in a single shot.

A prototype device capable of splitting an X-ray pulse into two adjustable fractions, delaying one of them with the aim of performing split pulse X-ray photon correlation spectroscopy and pump–probe type studies was designed and manufactured. Time delays up to 2.95 ns have been demonstrated. The achieved contrast values of 56% indicate a feasibility of performing coherence-based experiments with the delay line., A hard X-ray delay line capable of splitting and delaying single X-ray pulses has been developed with the aim of performing X-ray photon correlation spectroscopy (XPCS) and X-ray pump–probe experiments at hard X-ray free-electron laser sources. The performance of the device was tested with 8.39 keV synchrotron radiation. Time delays up to 2.95 ns have been demonstrated. The feasibility of the device for performing XPCS studies was tested by recording static speckle patterns. The achieved speckle contrast of 56% indicates the possibility of performing ultra-fast XPCS studies with the delay line.

In its 324 bunch‐mode of operation, the Advanced Photon Source (APS) has opened new avenues of femtosecond‐laser science and techniques. In this new mode, if one uses the tightly focused low‐pulse energy (nJ), high repetition rate fs‐laser Ti:sapphire oscillator (88 MHz) on beamline 7ID, every laser pulse and X‐ray bunch can be overlapped and delayed with respect to each other, resulting in a high‐repetition rate pump‐probe experiment that uses all the APS X‐ray bunches. This paper describes an example of how coherent X‐ray experiments may be used to study laser‐generated strain fields in semiconductors. With an oscillator beam focused to 6 μm onto GaAs, we have observed coherent X‐ray diffraction patterns with a high‐resolution camera. We have developed two techniques to observe the strain field, a topographic technique and a coherent diffraction technique. The topographic technique is quite useful to achieve a coarse spatial overlap of the the laser and X‐ray beams. The coherent X‐ray technique allows o...

The ability to synchronize a femtosecond laser to x-ray pulses is crucial for performing ultrafast time-resolved x-ray scattering experiments at synchrotrons. Conventionally, the task has been achieved by locking a harmonic frequency of the laser oscillator to the storage ring master radio-frequency (RF). However, when the frequency mismatch between the two sources cannot be compensated by small adjustments to the laser cavity length, synchronization to a harmonic frequency requires modifying the optical components of the laser system. We demonstrate a novel synchronization scheme, which is a flexible alternative for synchronizing these two sources operating at arbitrarily different frequencies. First, we find the greatest common divisor (GCD) of the two frequencies that is still within the limited tuning range of the laser cavity length. The GCD is generated by dividing down from the storage ring RF, and is separately multiplied up to provide a feedback signal for synchronizing the laser cavity. Unique to our scheme, the GCD also serves as a harmonic RF source for the laser amplifier such that only laser oscillator pulses at fixed integer multiples of the storage ring RF are selected for amplification and delivery to experiments. Our method is implemented at the Photon Test Facility beamline of Pohang Light Source where timing-jitter less than 4 ps (r.m.s.) is measured using a new shot-to-shot method.

We report an alternate light scattering approach to measure intermediate scattering function and structures of colloidal suspension by using two-pulse speckle contrast correlation analysis. By systematically controlling time-delays between two laser pulses incident on the sample, we are able to monitor transient evolution of coherent diffraction pattern, from which particle dynamics at different length and time scales are obtained simultaneously. Our result demonstrates the feasibility of utilizing a megapixel detector to achieve sufficient data statistics in a short amount of time while enabling microsecond time-resolution. Ultimately, this method provides means to measure high-speed dynamics well beyond the time response limit of a large area two-dimensional (2D) detector. (C) 2014 Optical Society of America

We describe the design and operation of a transmissive single-shot spectrometer for the measurement of hard x-ray free electron laser (FEL) source spectrum at the Linac Coherent Light Source (LCLS). The spectrometer was built around a 10 μm thick near-perfect silicon single crystal that was cylindrically bent. Its energy range covered the full FEL bandwidth while its resolution was sufficient for resolving single spectral spikes characteristics of the FELs. Its application will not only greatly facilitate the understanding and optimization of the x-ray FEL sources, but can also serve as an invaluable inline diagnostic tool for experiments where the spectral content of the source plays an important role in data interpretation.

We measured the relative arrival time between an optical pulse and a soft x-ray pulse from a free-electron laser. This femtosecond cross-correlation measurement was achieved by observing the change in optical reflectivity induced through the absorption of a fraction of the x-ray pulse. The main x-ray pulse energy remained available for an independent pump-probe experiment where the sample may be opaque to soft x-rays. The method was employed to correct the two-pulse delay data from a canonical pump-probe experiment and demonstrate 130 ± 20 fs (FWHM) temporal resolution. We further analyze possible timing jitter sources and point to future improvements.