Software defined photon counting system for time resolved x-ray experiments

The time structure of synchrotron radiation allows time resolved experiments with sub-100 ps temporal resolution using a pump-probe approach. However, the relaxation time of the samples may require a lower repetition rate of the pump pulse compared to the full repetition rate of the x-ray pulses from the synchrotron. The use of only the x-ray pulse immediately following the pump pulse is not efficient and often requires special operation modes where only a few buckets of the storage ring are filled. We designed a novel software defined photon counting system that allows to implement a variety of pump-probe schemes at the full repetition rate. The high number of photon counters allows to detect the response of the sample at multiple time delays simultaneously, thus improving the efficiency of the experiment. The system has been successfully applied to time resolved scanning transmission x-ray microscopy. However, this technique is applicable more generally.     

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.     

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.     

Multipurpose modular experimental station for the DiProI beamline of Fermi@Elettra free electron laser

We present a compact modular apparatus with a flexible design that will be operated at the DiProI beamline of the Fermi@Elettra free electron laser (FEL) for performing static and time-resolved coherent diffraction imaging experiments, taking advantage of the full coherence and variable polarization of the short seeded FEL pulses. The apparatus has been assembled and the potential of the experimental setup is demonstrated by commissioning tests with coherent synchrotron radiation. This multipurpose experimental station will be open to general users after installation at the Fermi@Elettra free electron laser in 2011.     

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.     

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.     

High repetition rate laser produced soft x-ray source for ultrafast x-ray absorption near edge structure measurements

Recent progress in high intensity ultrafast laser systems provides the opportunity to produce laser plasma x-ray sources exhibiting broad spectrum and high average x-ray flux that are well adapted to x-ray absorption measurements. In this paper, the development of a laser based x-ray absorption near edge structure (XANES) beamline exhibiting high repetition rate by using the Advanced Laser Light Source (ALLS) facility 100 Hz laser system (100 mJ, 35 fs at 800 nm) is presented. This system is based on a broadband tantalum solid target soft x-ray source and a grazing incidence grating spectrometer in the 1-5 nm wavelength range. To demonstrate the high potential of this laser based XANES technique in condensed matter physics, material science, or biology, measurements realized with several samples are presented: VO2 vanadium L edge, Si3N4 nitrogen K edge, and BPDA/PPD polyimide carbon K edge. The characteristics of this laser based beamline are discussed in terms of brightness, signal to noise ratio, and compared to conventional synchrotron broadband x-ray sources which allow achieving similar measurements. Apart from the very compact size and the relative low cost, the main advantages of such a laser based soft x-ray source are the picosecond pulse duration and the perfect synchronization between this x-ray probe and a laser pulse excitation which open the way to the realization of time resolved x-ray absorption measurements with picosecond range time resolution to study the dynamics of ultrafast processes and phase transition.     

Development of soft x-ray time-resolved photoemission spectroscopy system with a two-dimensional angle-resolved time-of-flight analyzer at SPring-8 BL07LSU

We have developed a soft x-ray time-resolved photoemission spectroscopy system using synchrotron radiation (SR) at SPring-8 BL07LSU and an ultrashort pulse laser system. Two-dimensional angle-resolved measurements were performed with a time-of-flight-type analyzer. The photoemission spectroscopy system is synchronized to light pulses of SR and laser using a time control unit. The performance of the instrument is demonstrated by mapping the band structure of a Si(111) crystal over the surface Brillouin zones and observing relaxation of the surface photo-voltage effect using the pump (laser) and probe (SR) method.     

Synchronized and configurable source of electrical pulses for x-ray pump-probe experiments

A method is described for the generation of software tunable patterns of nanosecond electrical pulses. The bipolar, high repetition rate (up to 250 MHz), fast rise time (<30 ps), square pulses are suitable for applications such as the excitation sequence in dynamic pump-probe experiments. Synchronization with the time structure of a synchrotron facility is possible as well as fine control of the relative delay in steps of 10 ps. The pulse generator described here is used to excite magnetic nanostructures with current pulses. Having an excitation system which can match the high repetition rate of a synchrotron allows for utilization of the full x-ray flux and is needed in experiments which require a large photon flux. The fast rise times allow for picosecond time resolution in pump-probe experiments. All pulse pattern parameters are configurable by software.     

X-ray diffraction in the pulsed laser heated diamond anvil cell

We have developed in situ x-ray synchrotron diffraction measurements of samples heated by a pulsed laser in the diamond anvil cell at pressure up to 60 GPa. We used an electronically modulated 2-10 kHz repetition rate, 1064-1075 nm fiber laser with 1-100 μs pulse width synchronized with a gated x-ray detector (Pilatus) and time-resolved radiometric temperature measurements. This enables the time domain measurements as a function of temperature in a microsecond time scale (averaged over many events, typically more than 10,000). X-ray diffraction data, temperature measurements, and finite element calculations with realistic geometric and thermochemical parameters show that in the present experimental configuration, samples 4 μm thick can be continuously temperature monitored (up to 3000 K in our experiments) with the same level of axial and radial temperature uniformities as with continuous heating. We find that this novel technique offers a new and convenient way of fine tuning the maximum sample temperature by changing the pulse width of the laser. This delicate control, which may also prevent chemical reactivity and diffusion, enables accurate measurement of melting curves, phase changes, and thermal equations of state.     

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 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.     

Versatile high-repetition-rate phase-locked chopper system for fast timing experiments in the vacuum ultraviolet and x-ray spectral region

A novel light chopper system for fast timing experiments in the vacuum-ultraviolet (VUV) and x-ray spectral region has been developed. It can be phase-locked and synchronized with a synchrotron radiation storage ring, accommodating repetition rates in the range of ~8 to ~120 kHz by choosing different sets of apertures and subharmonics of the ring frequency (MHz range). Also the opening time of the system can be varied from some nanoseconds to several microseconds to meet the needs of a broad range of applications. Adjusting these parameters, the device can be used either for the generation of single light pulses or pulse packages from a microwave driven, continuous He gas discharge lamp or from storage rings which are otherwise often considered as quasi-continuous light sources. This chopper can be utilized for many different kinds of experiments enabling, for example, unambiguous time-of-flight (TOF) multi-electron coincidence studies of atoms and molecules excited by a single light pulse as well as time-resolved visible laser pump x-ray probe electron spectroscopy of condensed matter in the valence and core level region.     

X-ray grating interferometer for materials-science imaging at a low-coherent wiggler source

X-ray phase-contrast radiography and tomography enable to increase contrast for weakly absorbing materials. Recently, x-ray grating interferometers were developed that extend the possibility of phase-contrast imaging from highly brilliant radiation sources like third-generation synchrotron sources to non-coherent conventional x-ray tube sources. Here, we present the first installation of a three grating x-ray interferometer at a low-coherence wiggler source at the beamline W2 (HARWI II) operated by the Helmholtz-Zentrum Geesthacht at the second-generation synchrotron storage ring DORIS (DESY, Hamburg, Germany). Using this type of the wiggler insertion device with a millimeter-sized source allows monochromatic phase-contrast imaging of centimeter sized objects with high photon flux. Thus, biological and materials-science imaging applications can highly profit from this imaging modality. The specially designed grating interferometer currently works in the photon energy range from 22 to 30 keV, and the range will be increased by using adapted x-ray optical gratings. Our results of an energy-dependent visibility measurement in comparison to corresponding simulations demonstrate the performance of the new setup.     

A multi-crystal wavelength dispersive x-ray spectrometer

A multi-crystal wavelength dispersive hard x-ray spectrometer with high-energy resolution and large solid angle collection is described. The instrument is specifically designed for time-resolved applications of x-ray emission spectroscopy (XES) and x-ray Raman scattering (XRS) at X-ray Free Electron Lasers (XFEL) and synchrotron radiation facilities. It also simplifies resonant inelastic x-ray scattering (RIXS) studies of the whole 2d RIXS plane. The spectrometer is based on the Von Hamos geometry. This dispersive setup enables an XES or XRS spectrum to be measured in a single-shot mode, overcoming the scanning needs of the Rowland circle spectrometers. In conjunction with the XFEL temporal profile and high-flux, it is a powerful tool for studying the dynamics of time-dependent systems. Photo-induced processes and fast catalytic reaction kinetics, ranging from femtoseconds to milliseconds, will be resolvable in a wide array of systems circumventing radiation damage.     

Time-resolved momentum imaging system for molecular dynamics studies using a tabletop ultrafast extreme-ultraviolet light source

We describe a momentum imaging setup for direct time-resolved studies of ionization-induced molecular dynamics. This system uses a tabletop ultrafast extreme-ultraviolet (EUV) light source based on high harmonic upconversion of a femtosecond laser. The high photon energy (around 42 eV) allows access to inner-valence states of a variety of small molecules via single photon excitation, while the sub--10-fs pulse duration makes it possible to follow the resulting dynamics in real time. To obtain a complete picture of molecular dynamics following EUV induced photofragmentation, we apply the versatile cold target recoil ion momentum spectroscopy reaction microscope technique, which makes use of coincident three-dimensional momentum imaging of fragments resulting from photoexcitation. This system is capable of pump-probe spectroscopy by using a combination of EUV and IR laser pulses with either beam as a pump or probe pulse. We report several experiments performed using this system.     

Continuous flow time-resolved small-angle x-ray scattering and X-ray absorption spectroscopy

A continuous flow device to characterize the growth of nanometer particles was assembled. In-situ millisecond or second-order time-resolved small angle x-ray scattering and x-ray absorption spectroscopy was performed using this device at the Beijing Synchrotron Radiation Facility. The time resolution was adjusted from 10 ms to 1.0 s by changing the flow rate of the solution. The temperature was variable from 5–95°C. Custom-designed pulse eliminators were employed to eliminate adverse pump fluctuations and improve the quality of measurements. The system was used to characterize zinc sulfide nanoparticles by small angle x-ray scattering and x-ray absorption spectroscopy.     

Continuous measurement of the arrival times of x-ray photon sequence

In order to record x-ray pulse profile for x-ray pulsar-based navigation and timing, this paper presents a continuous, high-precision method for measuring arrival times of photon sequence with a common starting point. In this method, a high stability atomic clock is counted to measure the coarse time of arrival photon. A high resolution time-to-digital converter is used to measure the fine time of arrival photon. The coarse times and the fine times are recorded continuously and then transferred to computer memory by way of memory switch. The pulse profile is obtained by a special data processing method. A special circuit was developed and a low-level x-ray pulse profile measurement experiment system was setup. The arrival times of x-ray photon sequence can be consecutively recorded with a time resolution of 500 ps and the profile of x-ray pulse was constructed. The data also can be used for analysis by many other methods, such as statistical distribution of photon events per time interval, statistical distribution of time interval between two photon events, photon counting histogram, autocorrelation and higher order autocorrelation.     

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.     

Femtosecond time-resolved photoelectron spectroscopy with a vacuum-ultraviolet photon source based on laser high-order harmonic generation

A laser-based tabletop approach to femtosecond time-resolved photoelectron spectroscopy with photons in the vacuum-ultraviolet (VUV) energy range is described. The femtosecond VUV pulses are produced by high-order harmonic generation (HHG) of an amplified femtosecond Ti:sapphire laser system. Two generations of the same setup and results from photoelectron spectroscopy in the gas phase are discussed. In both generations, a toroidal grating monochromator was used to select one harmonic in the photon energy range of 20-30 eV. The first generation of the setup was used to perform photoelectron spectroscopy in the gas phase to determine the bandwidth of the source. We find that our HHG source has a bandwidth of 140 ± 40 meV. The second and current generation is optimized for femtosecond pump-probe photoelectron spectroscopy with high flux and a small spot size at the sample of the femtosecond probe pulses. The VUV radiation is focused into the interaction region with a toroidal mirror to a spot smaller than 100 × 100 μm(2) and the flux amounts to 10(10) photons/s at the sample at a repetition rate of 1 kHz. The duration of the monochromatized VUV pulses is determined to be 120 fs resulting in an overall pump-probe time resolution of 135 ± 5 fs. We show how this setup can be used to map the transient valence electronic structure in molecular dissociation.