Spatial Distortion of Vibration Modes via Magnetic Correlation of Impurities.

Long wavelength vibrational modes in the ferromagnetic semiconductor Ga_{0.91}Mn_{0.09}As are investigated using time resolved x-ray diffraction. At room temperature, we measure oscillations in the x-ray diffraction intensity corresponding to coherent vibrational modes with well-defined wavelengths. When the correlation of magnetic impurities sets in, we observe the transition of the lattice into a disordered state that does not support coherent modes at large wavelengths. Our measurements point toward a magnetically induced broadening of long wavelength vibrational modes in momentum space and their quasilocalization in the real space. More specifically, long wavelength vibrational modes cannot be assigned to a single wavelength but rather should be represented as a superposition of plane waves with different wavelengths. Our findings have strong implications for the phonon-related processes, especially carrier-phonon and phonon-phonon scattering, which govern the electrical conductivity and thermal management of semiconductor-based devices.

Laboratory Setup for Scanning-Free Grazing Emission X-ray Fluorescence.

Grazing incidence and grazing emission X-ray fluorescence spectroscopy (GI/GE-XRF) are techniques that enable nondestructive, quantitative analysis of elemental depth profiles with a resolution in the nanometer regime. A laboratory setup for soft X-ray GEXRF measurements is presented. Reasonable measurement times could be achieved by combining a highly brilliant laser produced plasma (LPP) source with a scanning-free GEXRF setup, providing a large solid angle of detection. The detector, a pnCCD, was operated in a single photon counting mode in order to utilize its energy dispersive properties. GEXRF profiles of the Ni-Lα,ß line of a nickel-carbon multilayer sample, which displays a lateral (bi)layer thickness gradient, were recorded at several positions. Simulations of theoretical profiles predicted a prominent intensity minimum at grazing emission angles between 5° and 12°, depending strongly on the bilayer thickness of the sample. This information was used to retrieve the bilayer thickness gradient. The results are in good agreement with values obtained by X-ray reflectometry, conventional X-ray fluorescence and transmission electron microscopy measurements and serve as proof-of-principle for the realized GEXRF setup. The presented work demonstrates the potential of nanometer resolved elemental depth profiling in the soft X-ray range with a laboratory source, opening, for example, the possibility of in-line or even in situ process control in semiconductor industry.

Nanoscale spin reversal by non-local angular momentum transfer following ultrafast laser excitation in ferrimagnetic GdFeCo.

Ultrafast laser techniques have revealed extraordinary spin dynamics in magnetic materials that equilibrium descriptions of magnetism cannot explain. Particularly important for future applications is understanding non-equilibrium spin dynamics following laser excitation on the nanoscale, yet the limited spatial resolution of optical laser techniques has impeded such nanoscale studies. Here we present ultrafast diffraction experiments with an X-ray laser that probes the nanoscale spin dynamics following optical laser excitation in the ferrimagnetic alloy GdFeCo, which exhibits macroscopic all-optical switching. Our study reveals that GdFeCo displays nanoscale chemical and magnetic inhomogeneities that affect the spin dynamics. In particular, we observe Gd spin reversal in Gd-rich nanoregions within the first picosecond driven by the non-local transfer of angular momentum from larger adjacent Fe-rich nanoregions. These results suggest that a magnetic material's microstructure can be engineered to control transient laser-excited spins, potentially allowing faster (~ 1 ps) spin reversal than in present technologies.

Femtosecond dark-field imaging with an X-ray free electron laser.

The emergence of femtosecond diffractive imaging with X-ray lasers has enabled pioneering structural studies of isolated particles, such as viruses, at nanometer length scales. However, the issue of missing low frequency data significantly limits the potential of X-ray lasers to reveal sub-nanometer details of micrometer-sized samples. We have developed a new technique of dark-field coherent diffractive imaging to simultaneously overcome the missing data issue and enable us to harness the unique contrast mechanisms available in dark-field microscopy. Images of airborne particulate matter (soot) up to two microns in length were obtained using single-shot diffraction patterns obtained at the Linac Coherent Light Source, four times the size of objects previously imaged in similar experiments. This technique opens the door to femtosecond diffractive imaging of a wide range of micrometer-sized materials that exhibit irreproducible complexity down to the nanoscale, including airborne particulate matter, small cells, bacteria and gold-labeled biological samples.

Nanoplasma dynamics of single large xenon clusters irradiated with superintense x-ray pulses from the linac coherent light source free-electron laser.

The plasma dynamics of single mesoscopic Xe particles irradiated with intense femtosecond x-ray pulses exceeding 10(16) W/cm2 from the Linac Coherent Light Source free-electron laser are investigated. Simultaneous recording of diffraction patterns and ion spectra allows eliminating the influence of the laser focal volume intensity and particle size distribution. The data show that for clusters illuminated with intense x-ray pulses, highly charged ionization fragments in a narrow distribution are created and that the nanoplasma recombination is efficiently suppressed.

Compact pnCCD-based X-ray camera with high spatial and energy resolution: a color X-ray camera.

For many applications there is a requirement for nondestructive analytical investigation of the elemental distribution in a sample. With the improvement of X-ray optics and spectroscopic X-ray imagers, full field X-ray fluorescence (FF-XRF) methods are feasible. A new device for high-resolution X-ray imaging, an energy and spatial resolving X-ray camera, is presented. The basic idea behind this so-called "color X-ray camera" (CXC) is to combine an energy dispersive array detector for X-rays, in this case a pnCCD, with polycapillary optics. Imaging is achieved using multiframe recording of the energy and the point of impact of single photons. The camera was tested using a laboratory 30 µm microfocus X-ray tube and synchrotron radiation from BESSY II at the BAMline facility. These experiments demonstrate the suitability of the camera for X-ray fluorescence analytics. The camera simultaneously records 69,696 spectra with an energy resolution of 152 eV for manganese K(α) with a spatial resolution of 50 µm over an imaging area of 12.7 × 12.7 mm(2). It is sensitive to photons in the energy region between 3 and 40 keV, limited by a 50 µm beryllium window, and the sensitive thickness of 450 µm of the chip. Online preview of the sample is possible as the software updates the sums of the counts for certain energy channel ranges during the measurement and displays 2-D false-color maps as well as spectra of selected regions. The complete data cube of 264 × 264 spectra is saved for further qualitative and quantitative processing.

Energy-dispersive X-ray micro Laue diffraction on a bent gold nanowire.

This article reports on energy-dispersive micro Laue (µLaue) diffraction of an individual gold nanowire that was mechanically deformed in three-point bending geometry using an atomic force microscope. The nanowire deformation was investigated by scanning the focused polychromatic X-ray beam along the nanowire and recording µLaue diffraction patterns using an energy-sensitive pnCCD detector that permits measurement of the angular positions of the Laue spots and the energies of the diffracted X-rays simultaneously. The plastic deformation of the nanowire was shown by a bending of up to 3.0 ± 0.1°, a torsion of up to 0.3 ± 0.1° and a maximum deformation depth of 80 ± 5 nm close to the position where the mechanical load was applied. In addition, extended Laue spots in the vicinity of one of the clamping points indicated the storage of geometrically necessary dislocations with a density of 7.5 × 1013 m-2. While µLaue diffraction with a non-energy-sensitive detector only gives access to the deviatoric strain, the energy sensitivity of the employed pnCCD offers absolute strain measurements with a resolution of 1%. Here, the residual strain after complete unloading of the nanowire amounted to maximum tensile and compressive strains of the order of +1.2 and -3%, which is comparable to the actual resolution limit. The combination of white-beam µLaue diffraction using an energy-sensitive pixel detector with nano-mechanical testing opens up new possibilities for the study of mechanical behavior at the nanoscale.

Towards ultrafast dynamics with split-pulse X-ray photon correlation spectroscopy at free electron laser sources.

One of the important challenges in condensed matter science is to understand ultrafast, atomic-scale fluctuations that dictate dynamic processes in equilibrium and non-equilibrium materials. Here, we report an important step towards reaching that goal by using a state-of-the-art perfect crystal based split-and-delay system, capable of splitting individual X-ray pulses and introducing femtosecond to nanosecond time delays. We show the results of an ultrafast hard X-ray photon correlation spectroscopy experiment at LCLS where split X-ray pulses were used to measure the dynamics of gold nanoparticles suspended in hexane. We show how reliable speckle contrast values can be extracted even from very low intensity free electron laser (FEL) speckle patterns by applying maximum likelihood fitting, thus demonstrating the potential of a split-and-delay approach for dynamics measurements at FEL sources. This will enable the characterization of equilibrium and, importantly also reversible non-equilibrium processes in atomically disordered materials.

Single-shot full strain tensor determination with microbeam X-ray Laue diffraction and a two-dimensional energy-dispersive detector.

The full strain and stress tensor determination in a triaxially stressed single crystal using X-ray diffraction requires a series of lattice spacing measurements at different crystal orientations. This can be achieved using a tunable X-ray source. This article reports on a novel experimental procedure for single-shot full strain tensor determination using polychromatic synchrotron radiation with an energy range from 5 to 23 keV. Microbeam X-ray Laue diffraction patterns were collected from a copper micro-bending beam along the central axis (centroid of the cross section). Taking advantage of a two-dimensional energy-dispersive X-ray detector (pnCCD), the position and energy of the collected Laue spots were measured for multiple positions on the sample, allowing the measurement of variations in the local microstructure. At the same time, both the deviatoric and hydrostatic components of the elastic strain and stress tensors were calculated.

A liquid jet setup for x-ray scattering experiments on complex liquids at free-electron laser sources.

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.

High-Resolution X-ray Spectroscopy Close to Room Temperature.

: Originally designed as position-sensitive detectors for particle tracking, silicon drift detectors (SDDs) are now used for high-count rate X-ray spectroscopy, operating close to room temperature. Their low-capacitance read-node concept places them among the fastest high-resolution detector systems. They have been used in a new spectrum of experiments in the wide field of X-ray spectroscopy: fluorescent analysis, diffractometry, materials analysis, and synchrotron experiments such as X-ray holography and element imaging in scanning electron microscopes. The fact that the detector system can be used at room temperature with good spectroscopic performance and at -10 degrees C with excellent energy resolution, avoiding liquid nitrogen for cooling and high-quality vacuum, guarantees a large variety of new applications, independent of the laboratory environment. A brief description of the device principles is followed by basics on low noise amplification. The performance results of a complete detector system are presented as well as some dedicated applications already realized, including use in a surface mapping instrument and use of a "mini-spectrometer" for the analysis of works of art. Fully depleted pn-charge-coupled devices (pn-CCDs) have been fabricated for the European X-ray Multi-Mirror mission (XMM) and the German X-ray satellite ABRIXAS, enabling high-speed, low-noise, position-resolving X-ray spectroscopy. The detector was designed and fabricated with a homogeneously sensitive area of 36 cm2. At -70 degrees C it has a noise of 4 e- rms, with a readout time of the total focal plane array of 4 msec. The maximum count rate for single photon counting was 10(5) cps under flat field conditions. In the integration mode, more than 10(9) cps can be detected at 6 keV. Its position resolution is on the order of 100 µm. The quantum efficiency is higher than 90%, ranging from carbon K X-rays (277 eV) up to 10 keV.

A new method for polychromatic X-ray µLaue diffraction on a Cu pillar using an energy-dispersive pn-junction charge-coupled device.

µLaue diffraction with a polychromatic X-ray beam can be used to measure strain fields and crystal orientations of micro crystals. The hydrostatic strain tensor can be obtained once the energy profile of the reflections is measured. However, this remains a challenge both on the time scale and reproducibility of the beam position on the sample. In this review, we present a new approach to obtain the spatial and energy profiles of Laue spots by using a pn-junction charge-coupled device, an energy-dispersive area detector providing 3D resolution of incident X-rays. The morphology and energetic structure of various Bragg peaks from a single crystalline Cu micro-cantilever used as a test system were simultaneously acquired. The method facilitates the determination of the Laue spots' energy spectra without filtering the white X-ray beam. The synchrotron experiment was performed at the BM32 beamline of ESRF using polychromatic X-rays in the energy range between 5 and 25 keV and a beam size of 0.5 µm × 0.5 µm. The feasibility test on the well known system demonstrates the capabilities of the approach and introduces the "3D detector method" as a promising tool for material investigations to separate bending and strain for technical materials.

Single-particle structure determination by correlations of snapshot X-ray diffraction patterns.

Diffractive imaging with free-electron lasers allows structure determination from ensembles of weakly scattering identical nanoparticles. The ultra-short, ultra-bright X-ray pulses provide snapshots of the randomly oriented particles frozen in time, and terminate before the onset of structural damage. As signal strength diminishes for small particles, the synthesis of a three-dimensional diffraction volume requires simultaneous involvement of all data. Here we report the first application of a three-dimensional spatial frequency correlation analysis to carry out this synthesis from noisy single-particle femtosecond X-ray diffraction patterns of nearly identical samples in random and unknown orientations, collected at the Linac Coherent Light Source. Our demonstration uses unsupported test particles created via aerosol self-assembly, and composed of two polystyrene spheres of equal diameter. The correlation analysis avoids the need for orientation determination entirely. This method may be applied to the structural determination of biological macromolecules in solution.

The DRAGO gamma camera.

In this work, we present the results of the experimental characterization of the DRAGO (DRift detector Array-based Gamma camera for Oncology), a detection system developed for high-spatial resolution gamma-ray imaging. This camera is based on a monolithic array of 77 silicon drift detectors (SDDs), with a total active area of 6.7 cm(2), coupled to a single 5-mm-thick CsI(Tl) scintillator crystal. The use of an array of SDDs provides a high quantum efficiency for the detection of the scintillation light together with a very low electronics noise. A very compact detection module based on the use of integrated readout circuits was developed. The performances achieved in gamma-ray imaging using this camera are reported here. When imaging a 0.2 mm collimated (57)Co source (122 keV) over different points of the active area, a spatial resolution ranging from 0.25 to 0.5 mm was measured. The depth-of-interaction capability of the detector, thanks to the use of a Maximum Likelihood reconstruction algorithm, was also investigated by imaging a collimated beam tilted to an angle of 45 degrees with respect to the scintillator surface. Finally, the imager was characterized with in vivo measurements on mice, in a real preclinical environment.

Differential phase contrast with a segmented detector in a scanning X-ray microprobe.

Scanning X-ray microprobes are unique tools for the nanoscale investigation of specimens from the life, environmental, materials and other fields of sciences. Typically they utilize absorption and fluorescence as contrast mechanisms. Phase contrast is a complementary technique that can provide strong contrast with reduced radiation dose for weakly absorbing structures in the multi-keV range. In this paper the development of a segmented charge-integrating silicon detector which provides simultaneous absorption and differential phase contrast is reported. The detector can be used together with a fluorescence detector for the simultaneous acquisition of transmission and fluorescence data. It can be used over a wide range of photon energies, photon rates and exposure times at third-generation synchrotron radiation sources, and is currently operating at two beamlines at the Advanced Photon Source. Images obtained at around 2 keV and 10 keV demonstrate the superiority of phase contrast over absorption for specimens composed of light elements.

Silicon drift detectors with on-chip electronics for x-ray spectroscopy.

The silicon drift detector (SDD) is a semiconductor device based on high resistivity silicon fully depleted through junctions implanted on both sides of the semiconductor wafer. The electrons generated by the ionizing radiation are driven by means of a suitable electric field from the point of interaction toward a collecting anode of small capacitance, independent of the active area of the detector. A suitably designed front-end JFET has been directly integrated on the detector chip close to the anode region, in order to obtain a nearly ideal capacitive matching between detector and transistor and to minimize the stray capacitances of the connections. This feature allows it to reach high energy resolution also at high count rates and near room temperature. The present work describes the structure and the performance of SDDs specially designed for high resolution spectroscopy with soft x rays at high detection rate. Experimental results of SDDs used in spectroscopy applications are also reported.

High-Resolution High-Count-Rate X-ray Spectroscopy with State-of-the-Art Silicon Detectors.

For the European X-ray multi-mirror (XMM) satellite mission and the German X-ray satellite ABRIXAS, fully depleted pn-CCDs have been fabricated, enabling high-speed low-noise position-resolving X-ray spectroscopy. The detector was designed and fabricated with a homogeneously sensitive area of 36 cm(2). At 150 K it has a noise of 4 e(-) r.m.s., with a readout time of the total focal plane array of 4 ms. The maximum count rate for single-photon counting was 10(5) counts s(-1) under flat-field conditions. In the integration mode more than 10(9) counts s(-1) can be detected at 6 keV. Its position resolution is of the order of 100 micro m. The quantum efficiency is higher than 90% from carbon K X-rays (277 eV) up to 10 keV. New cylindrical silicon drift detectors have been designed, fabricated and tested. They comprise an integrated on-chip amplifier system with continuous reset, on-chip voltage divider, electron accumulation layer stabilizer, large area, homogeneous radiation entrance window and a drain for surface-generated leakage current. At count rates as high as 2 x 10(6) counts cm(-2) s(-1), they still show excellent spectroscopic behaviour at room-temperature operation in single-photon detection mode. The energy resolution at room temperature is 220 eV at 6 keV X-ray energy and 140 eV at 253 K, being achieved with Peltier coolers. These systems were operated at synchrotron light sources (ESRF, HASYLAB and NLS) as X-ray fluorescence spectrometers in scanning electron microscopes and as ultra low noise photodiodes. The operation of a multi-channel silicon drift detector system is already foreseen at synchrotron light sources for X-ray holography experiments. All systems are fabricated in planar technology having the detector and amplifiers monolithically integrated on high-resistivity silicon.