Development of high-repetition-rate laser pump/x-ray probe methodologies for synchrotron facilities

We describe our implementation of a high repetition rate (54 kHz-6.5 MHz), high power (>10 W), laser system at the 7ID beamline at the Advanced Photon Source for laser pump/x-ray probe studies of optically driven molecular processes. Laser pulses at 1.06 μm wavelength and variable duration (10 or 130 ps) are synchronized to the storage ring rf signal to a precision of ~250 fs rms. Frequency doubling and tripling of the laser radiation using nonlinear optical techniques have been applied to generate 532 and 355 nm light. We demonstrate that by combining a microfocused x-ray probe with focused optical laser radiation the requisite fluence (with <10 μJ/pulse) for efficient optical excitation can be readily achieved with a compact and commercial laser system at megahertz repetition rates. We present results showing the time-evolution of near-edge x-ray spectra of a well-studied, laser-excited metalloporphyrin, Ni(II)-tetramesitylporphyrin. The use of high repetition rate, short pulse lasers as pump sources will dramatically enhance the duty cycle and efficiency in data acquisition and hence capabilities for laser-pump/x-ray probe studies of ultrafast structural dynamics at synchrotron sources.     

Time-resolved soft x-ray absorption setup using multi-bunch operation modes at synchrotrons

Here, we report on a novel experimental apparatus for performing time-resolved soft x-ray absorption spectroscopy in the sub-ns time scale using non-hybrid multi-bunch mode synchrotron radiation. The present setup is based on a variable repetition rate Ti:sapphire laser (pump pulse) synchronized with the ~500 MHz x-ray synchrotron radiation bunches and on a detection system that discriminates and singles out the significant x-ray photon pulses by means of a custom made photon counting unit. The whole setup has been validated by measuring the time evolution of the L(3) absorption edge during the melting and the solidification of a Ge single crystal irradiated by an intense ultrafast laser pulse. These results pave the way for performing synchrotron time-resolved experiments in the sub-ns time domain with variable repetition rate exploiting the full flux of the synchrotron radiation.     

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.     

Gas gun shock experiments with single-pulse x-ray phase contrast imaging and diffraction at the Advanced Photon Source

The highly transient nature of shock loading and pronounced microstructure effects on dynamic materials response call for in situ, temporally and spatially resolved, x-ray-based diagnostics. Third-generation synchrotron x-ray sources are advantageous for x-ray phase contrast imaging (PCI) and diffraction under dynamic loading, due to their high photon fluxes, high coherency, and high pulse repetition rates. The feasibility of bulk-scale gas gun shock experiments with dynamic x-ray PCI and diffraction measurements was investigated at the beamline 32ID-B of the Advanced Photon Source. The x-ray beam characteristics, experimental setup, x-ray diagnostics, and static and dynamic test results are described. We demonstrate ultrafast, multiframe, single-pulse PCI measurements with unprecedented temporal (<100 ps) and spatial (～2 μm) resolutions for bulk-scale shock experiments, as well as single-pulse dynamic Laue diffraction. The results not only substantiate the potential of synchrotron-based experiments for addressing a variety of shock physics problems, but also allow us to identify the technical challenges related to image detection, x-ray source, and dynamic loading.     

A high-repetition rate scheme for synchrotron-based picosecond laser pump/x-ray probe experiments on chemical and biological systems in solution

We present the extension of time-resolved optical pump/x-ray absorption spectroscopy (XAS) probe experiments towards data collection at MHz repetition rates. The use of a high-power picosecond laser operating at an integer fraction of the repetition rate of the storage ring allows exploitation of up to two orders of magnitude more x-ray photons than in previous schemes based on the use of kHz lasers. Consequently, we demonstrate an order of magnitude increase in the signal-to-noise of time-resolved XAS of molecular systems in solution. This makes it possible to investigate highly dilute samples at concentrations approaching physiological conditions for biological systems. The simplicity and compactness of the scheme allows for straightforward implementation at any synchrotron beamline and for a wide range of x-ray probe techniques, such as time-resolved diffraction or x-ray emission studies.     

A tabletop femtosecond time-resolved soft x-ray transient absorption spectrometer

A laser-based, tabletop instrument is constructed to perform femtosecond soft x-ray transient absorption spectroscopy. Ultrashort soft x-ray pulses produced via high-order harmonic generation of the amplified output of a femtosecond Ti:sapphire laser system are used to probe atomic core-level transient absorptions in atoms and molecules. The results provide chemically specific, time-resolved dynamics with sub-50-fs time resolution. In this setup, high-order harmonics generated in a Ne-filled capillary waveguide are refocused by a gold-coated toroidal mirror into the sample gas cell, where the soft x-ray light intersects with an optical pump pulse. The transmitted high-order harmonics are spectrally dispersed with a homebuilt soft x-ray spectrometer, which consists of a gold-coated toroidal mirror, a uniform-line spaced plane grating, and a soft x-ray charge coupled device camera. The optical layout of the instrument, design of the soft x-ray spectrometer, and spatial and temporal characterizations of the high-order harmonics are described. Examples of static and time-resolved photoabsorption spectra collected on this apparatus are presented.     

Synchrotron-based ultrafast x-ray diffraction at high repetition rates

We present a setup for ultrafast x-ray diffraction (UXRD) based at the storage ring BESSY II, in particular, a pump laser that excites the sample using 250 fs laser-pulses at repetition rates ranging from 208 kHz to 1.25 MHz. We discuss issues connected to the high heat-load and spatio-temporal alignment strategies in the context of a UXRD experiment at high repetition rates. The spatial overlap between laser pump and x-ray probe pulse is obtained with 10 μm precision and transient lattice changes can be recorded with an accuracy of δa/a(0) = 10(-6). We also compare time-resolved x-ray diffraction signals from a laser excited LSMO/STO superlattice with phonon dynamics simulations. From the analysis we determine the x-ray pulse duration to 120 ps in standard operation mode and below 10 ps in low-α mode.     

Variable rowland radius laboratory vacuum surface-sensitive x-ray absorption fine structure spectrometer

A new laboratory x-ray spectrometer for surface-sensitive extended x-ray absorption fine structure [(S)EXAFS] and surface-sensitive x-ray absorption near-edge structure [(S)XANES] measurements is described. The spectrometer employs a 12 kV mA rotating anode generator. It has a monochromator equipped with a set of exchangeable curved crystals of Johann or Johansson type with different cell parameters, orientations, and Rowland radii. The computer controlled movement system based on nine stepping motors allows all the main elements of the spectrometer to be positioned freely relative to the x-ray source and gives an opportunity to use sophisticated scanning modes (for example, a mode with a focus spot position on a sample surface instead of an exit slit). The whole x-ray beam line is completely enclosed in a vacuum chamber that is directly connected to the x-ray generator, thereby preventing the absorption of x rays in the air. This layout allows a wide x-ray photon energy range from a few keV up to dozens of keV. A registration of x rays transmitted through the sample with proportional counter- and photoelectrons emitted from the sample with channeltron is used to carry out bulk- and surface-sensitive measurements, respectively. Using a 25 x 200 kV mA power regime of a rotating anode x-ray generator, a photon flux of 2.5 x 10(5) counts/s was registered at the Cu K edge, where the energy resolution was about 5 eV. High near surface sensitivity is demonstrated by the EXAFS spectra of Cu K and Hf LIII edges measured from 3 nm Cu and Hf oxide films.     

Time-resolved near-edge x-ray absorption fine structure spectroscopy on photo-induced phase transitions using a tabletop soft-x-ray spectrometer

We present a table-top soft-x-ray spectrometer for the wavelength range λ = 1-5 nm based on a stable laser-driven x-ray source, making use of a gas-puff target. With this setup, optical light-pump/soft-x-ray probe near-edge x-ray absorption fine structure (NEXAFS) experiments with a temporal resolution of about 230 ps are feasible. Pump-probe NEXAFS measurements were carried out in the "water-window" region (2.28 nm-4.36 nm) on the manganite Pr(0.7)Ca(0.3)MnO(3), investigating diminutive changes of the oxygen K edge that derive from an optically induced phase transition. The results show the practicability of the table-top soft-x-ray spectrometer on demanding investigations so far exclusively conducted at synchrotron radiation sources.     

KMC-1: a high resolution and high flux soft x-ray beamline at BESSY

The crystal monochromator beamline KMC-1 at a BESSY II bending magnet covers the energy range from soft (1.7 keV) to hard x-rays (12 keV) employing the (n,-n) double crystal arrangement with constant beam offset. The monochromator is equipped with three sets of crystals, InSb, Si (111), and Si (422) which are exchangeable in situ within a few minutes. Beamline and monochromator have been optimized for high flux and high resolution. This could be achieved by (1) a windowless setup under ultrahigh-vacuum conditions up to the experiment, (2) by the use of only three optical elements to minimize reflection losses, (3) by collecting an unusually large horizontal radiation fan (6 mrad) with the toroidal premirror, and (4) the optimization of the crystal optics to the soft x-ray range necessitating quasibackscattering crystal geometry (theta(Bragg,max)=82 degrees) delivering crystal limited resolution. The multipurpose beamline is in use for a variety of user facilities such as extended x-ray absorption fine structure, ((Bio-)EXAFS) near-edge x-ray absorption fine structure (NEXAFS), absorption and fluorescence spectroscopy. Due to the windowless UHV setup the k edges of the technologically and biologically important elements such as Si, P, and S are accessible. In addition to these experiments this beamline is now extensively used for photoelectron spectroscopy at high kinetic energies. Photon flux in the 10(11)-10(12) photons/s range and beamline resolving powers of more than E/DeltaE approximately 100.000 have been measured at selected energies employing Si (nnn) high order radiation in quasibackscattering geometry, thus photoelectron spectroscopy with a total instrumental resolution of about 150 meV is possible. This article describes the design features of the beamline and reports some experimental results in the above mentioned fields.     

High-performance soft x-ray spectromicroscopy beamline at SSRF

The Shanghai Synchrotron Radiation Facility (SSRF) is the first third-generation synchrotron facility in China and operated at an electron energy of 3.5 GeV. One of the seven beamlines in the first construction phase is devoted to soft x-ray spectromicroscopy and is equipped with an elliptically polarized undulator light source, a plane grating monochromator, and a scanning transmission x-ray microscope end station. Initial results reveal the high performance of this beamline, with an energy resolving power estimated to be over 10,000 at the argon L-edge and a spatial resolution better than 30 nm.     

Miniature pulsed magnet system for synchrotron x-ray measurements

We have developed a versatile experimental apparatus for synchrotron x-ray measurements in pulsed high magnetic fields. The apparatus consists of a double cryostat incorporating a liquid nitrogen bath to cool the miniature pulsed coil and an independent helium flow cryostat allowing sample temperatures from 4 up to 250 K. The high duty cycle miniature pulsed coils can generate up to 38 T. During experiments at 30 T a repetition rate of 6 pulsesmin was routinely reached. Using a 4 kJ power supply, the pulse duration was between 500 mus and 1 ms. The setup was used for nuclear forward scattering measurements on 57Fe up to 25 T on the ESRF beamline ID18. In another experiment, x-ray magnetic circular dichroism was measured up to 30 T on the ESRF energy dispersive beamline ID24.     

Construction and development of a time-resolved x-ray magnetic circular dichroism-photoelectron emission microscopy system using femtosecond laser pulses at BL25SU SPring-8

A femtosecond pulsed laser system has been installed at the BL25SU soft x-ray beamline at SPring-8 for time-resolved pump-probe experiments with synchronization of the laser pulses to the circularly polarized x-ray pulses. There are four different apparatuses situated at the beamline; for photoemission spectroscopy, two-dimensional display photoelectron diffraction, x-ray magnetic circular dichroism (XMCD) with electromagnetic coils, and photoelectron emission microscopy (PEEM). All four can be used for time-resolved experiments, and preliminary investigations have been carried out using the PEEM apparatus to observe magnetization dynamics in combination with XMCD. In this article, we describe the details of the stroboscopic pump-probe XMCD-PEEM experiment, and present preliminary data. The repetition rate of the laser pulses is set using a pulse selector to match the single bunches of SPring-8's hybrid filling pattern, which consists of several single bunches and a continuous bunch train. Electrons ejected during the bunch train, which do not provide time-resolved signal, are eliminated by periodically reducing the channel plate voltage using a custom-built power supply. The pulsed laser is used to create 300 ps long magnetic field pulses, which cause magnetic excitations in micron-sized magnetic elements which contain magnetic vortex structures. The observed frequency of the motion is consistent with previously reported observations and simulations.     

Application of a transmission crystal x-ray spectrometer to moderate-intensity laser driven sources

In the pursuit of novel, laser-produced x-ray sources for medical imaging applications, appropriate instrumental diagnostics need to be developed concurrently. A type of transmission crystal spectroscopy has previously been demonstrated as a survey tool for sources produced by high-power and high-energy lasers. The present work demonstrates the extension of this method into the study of medium-intensity laser driven hard x-ray sources with a design that preserves resolving power while maintaining high sensitivity. Specifically, spectroscopic measurements of characteristic Kα and Kβ emissions were studied from Mo targets irradiated by a 100 fs, 200 mJ, Ti: sapphire laser with intensity of 10(17) W/cm(2) to 10(18) W∕cm(2) per shot. Using a transmission curved crystal spectrometer and off-Rowland circle imaging, resolving powers (E/ΔE) of around 300 for Mo Kα(2) at 17.37 keV were obtained with an end-to-end spectrometer efficiency of (1.13 ± 0.10) × 10(-5). This sensitivity is sufficient for registering x-ray lines with high signal to background from targets following irradiation by a single laser pulse, demonstrating the utility of this method in the study of the development of medium-intensity laser driven x-ray sources.     

Ultra-high-precision time control system over any long time delay for laser pump and synchrotron x-ray probe experiment

An ultra-high-precision clock system for long time delay has been developed for picosecond time-resolved x-ray diffraction measurements using synchrotron radiation (SR) pulses and synchronized femtosecond laser pulses. The time delay control between pump laser pulse and the probe SR pulse was achieved by combining an in-phase quadrature modulator and a synchronous counter. This method allowed us to change the delay time by a nearly infinite amount while maintaining the precision of +/-8.40 ps. Time-resolved diffraction measurements using the delay control system were demonstrated for precise measurement of an acoustic velocity in a single crystal of gallium arsenide.     

A broadband laser plasma x-ray source for application in ultrafast chemical structure dynamics

A plasma source free from characteristic emission lines is described, based on laser irradiation of a water jet in a helium atmosphere. Various key aspects of the laser interaction are presented along with practical characterization of the observed isotropic approximately 4-10 keV x-ray emissions, measurements of which indicate subpicosecond duration. Observations are consistent with a vacuum heating plasma mechanism at the helium-water interface and indicate strong potential for in-house ultrafast chemical structure dynamics application when coupled to contemporary detector developments.     

Note: Optical trigger device with sub-picosecond timing jitter and stability

We are presenting the design, construction, and overall performance of the optical trigger device. This device generates an electrical signal synchronously to the detected ultra-short optical pulse. The device was designed for application in satellite laser ranging and laser time transfer experiments, time correlated photon counting and similar experiments, where picosecond timing resolution and detection delay stability are required. It consists of the ultrafast optical detector, signal discriminator, output pulse forming circuit, and output driver circuits. It was constructed as a single compact device to optimize their matching and maintain stability. The detector consists of an avalanche photodiode--both silicon and germanium types may be used to cover the wavelength range of 350-1550 nm. The analogue signal of this photodiode is sensed by the ultrafast comparator with 8 GHz bandwidth. The ps clock distribution circuit is used to generate the fast rise/fall time output pulses of pre-set length. The trigger device timing performance is excellent: the random component of the timing jitter is typically 880 fs, the temperature dependence of the detection delay was measured to be 370 fs/K. The systematic error contribution depends on the laser used and its stability. The sub-ps values have been obtained for various laser sources.     

Development of a time-resolved soft x-ray spectrometer for laser produced plasma experiments

A 2400 lines/mm variable-spaced grating spectrometer has been used to measure soft x-ray emission (8-22 A?) from laser-produced plasma experiments at Lawrence Livermore National Laboratory's Compact Multipulse Terrawatt (COMET) Laser Facility. The spectrometer was coupled to a Kentech x-ray streak camera to study the temporal evolution of soft x rays emitted from the back of the Mylar and the copper foils irradiated at 10(15)?W/cm(2). The instrument demonstrated a resolving power of ～120 at 19 A? with a time resolution of 31 ps. The time-resolved copper emission spectrum was consistent with a photodiode monitoring the laser temporal pulse shape and indicated that the soft x-ray emission follows the laser heating of the target. The time and spectral resolutions of this diagnostic make it useful for studies of high temperature plasmas.     

A sample holder for soft x-ray absorption spectroscopy of liquids in transmission mode

A novel sample holder for soft x-ray absorption spectroscopy of liquids in transmission mode based on sample cells with x-ray transparent silicon nitride membranes is introduced. The sample holder allows for a reliable preparation of ultrathin liquid films with an adjustable thickness in the nm-μm range. This enables measurements of high quality x-ray absorption spectra of liquids in transmission mode, as will be shown for the example of liquid H(2)O, aqueous solutions of 3d-transition metal ions and alcohol-water mixtures. The fine structure of the x-ray absorption spectra is not affected by the sample thickness. No effects of the silicon nitride membranes were observed in the spectra. It is shown how an inhomogeneous thickness of the sample affects the spectra and how this can be avoided.     

An in-vacuum x-ray diffraction microscope for use in the 0.7-2.9 keV range

A dedicated in-vacuum coherent x-ray diffraction microscope was installed at the 2-ID-B beamline of the Advanced Photon Source for use with 0.7-2.9 keV x-rays. The instrument can accommodate three common implementations of diffractive imaging; plane wave illumination; defocused-probe (Fresnel diffractive imaging) and scanning (ptychography) using either a pinhole, focused or defocused probe. The microscope design includes active feedback to limit motion of the optics with respect to the sample. Upper bounds on the relative optics-to-sample displacement have been measured to be 5.8 nm(v) and 4.4 nm(h) rms/h using capacitance micrometry and 27 nm/h using x-ray point projection imaging. The stability of the measurement platform and in-vacuum operation allows for long exposure times, high signal-to-noise and large dynamic range two-dimensional intensity measurements to be acquired. Finally, we illustrate the microscope's stability with a recent experimental result.