Third-generation Synchrotron Radiation Sources Research Articles

High-resolution electron time-of-flight spectrometers for angle-resolved measurements at the SQS Instrument at the European XFEL.

A set of electron time-of-flight spectrometers for high-resolution angle-resolved spectroscopy was developed for the Small Quantum Systems (SQS) instrument at the SASE3 soft X-ray branch of the European XFEL. The resolving power of this spectrometer design is demonstrated to exceed 10 000 (E/ΔE), using the well known Ne 1s-13p resonant Auger spectrum measured at a photon energy of 867.11 eV at a third-generation synchrotron radiation source. At the European XFEL, a width of ∼0.5 eV full width at half-maximum for a kinetic energy of 800 eV was demonstrated. It is expected that this linewidth can be reached over a broad range of kinetic energies. An array of these spectrometers, with different angular orientations, is tailored for the Atomic-like Quantum Systems endstation for high-resolution angle-resolved spectroscopy of gaseous samples.

X-ray magnetic diffraction under high pressure.

Advances in both non-resonant and resonant X-ray magnetic diffraction since the 1980s have provided researchers with a powerful tool for exploring the spin, orbital and ion degrees of freedom in magnetic solids, as well as parsing their interplay. Here, we discuss key issues for performing X-ray magnetic diffraction on single-crystal samples under high pressure (above 40 GPa) and at cryogenic temperatures (4 K). We present case studies of both non-resonant and resonant X-ray magnetic diffraction under pressure for a spin-flip transition in an incommensurate spin-density-wave material and a continuous quantum phase transition of a commensurate all-in-all-out antiferromagnet. Both cases use diamond-anvil-cell technologies at third-generation synchrotron radiation sources. In addition to the exploration of the athermal emergence and evolution of antiferromagnetism discussed here, these techniques can be applied to the study of the pressure evolution of weak charge order such as charge-density waves, antiferro-type orbital order, the charge anisotropic tensor susceptibility and charge superlattices associated with either primary spin order or softened phonons.

Experimental setup for the study of resonant inelastic X-ray scattering of organometallic complexes in gas phase.

A new setup has been designed and built to study organometallic complexes in gas phase at the third-generation Synchrotron radiation sources. This setup consists of a new homemade computer-controlled gas cell that allows us to sublimate solid samples by accurately controlling the temperature. This cell has been developed to be a part of the high-resolution X-ray emission spectrometer permanently installed at the GALAXIES beamline of the French National Synchrotron Facility SOLEIL. To illustrate the capabilities of the setup, the cell has been successfully used to record high-resolution Kα emission spectra of gas-phase ferrocene Fe(C5H5)2 and to characterize their dependence with the excitation energy. This will allow to extend resonant X-ray emission to different organometallic molecules.

Studies of electron diffusion in photo-excited Ni using time-resolved X-ray diffraction

We show that the heat deposition profile in a laser-excited metal can be determined by time-resolved X-ray diffraction. In this study, we investigated the electron diffusion in a 150 nm thick nickel film deposited on an indium antimonide substrate. A strain wave that mimics the heat deposition profile is generated in the metal and propagates into the InSb, where it influences the temporal profile of X-rays diffracted from InSb. We found that the strain pulse significantly deviated from a simple exponential profile, and that the two-temperature model was needed to reproduce the measured heat deposition profile. Experimental results were compared to simulations based on the two-temperature model carried out using commercial finite-element software packages and on-line dynamical diffraction tools. To reproduce the experimental data, the electron–phonon coupling factor was lowered compared to previously measured values. The experiment was carried out at a third-generation synchrotron radiation source using a ...

Advances in high-resolution RIXS for the study of excitation spectra under high pressure

ABSTRACTHard X-ray resonant inelastic X-ray scattering (RIXS) is a promising X-ray spectroscopic tool for measuring low-energy excitation spectra from complex materials under high pressure. In the past, these measurements have been stymied by technical difficulties inherent in measuring a tiny sample, held at high pressure, inside a diamond anvil cell. Now, due to substantial advances in X-ray instrumentation, high-resolution ( meV) RIXS spectrometers at third-generation synchrotron radiation sources have started to successfully address these samples in their extreme environment. However, compared to elastic X-ray scattering and X-ray emission spectroscopy, RIXS is a very photon hungry technique and high-resolution RIXS for samples under high pressure is in its infancy. In this review, the fundamentals of the high-resolution RIXS and associated instrumentation are presented, as well as technical details of diamond anvil cells, sample preparation, and the measurement geometry. Experimental data from measurements of 3d- and 5d-transition metal oxides are shown and future improvements of the RIXS technique in the context of high pressure are discussed.

Present research status of piezoelectric bimorph mirrors in synchrotron radiation sources

The third-generation synchrotron radiation sources are widely used in physics, chemistry, material science, etc. due to their light beams with high brilliance and low emittance. In order to efficiently utilize such light beams for scientific research, reflective mirrors with excellent figure quality are required. The reflective mirrors on the beamlines of synchrotron radiation sources consist of fixed polished shape mirrors and bendable mirrors. Bendable mirrors have been attracting the attention of the synchrotron radiation community because their curvatures can be varied to realize different focusing properties. Classical bendable mirrors are realized by applying mechanical moment at the ends of the mirror substrates. In this paper, we introduce a new concept of bendable mirrors, X-ray adaptive mirrors which are based on the adaptive optics technology and the properties of piezoelectric bimorph systems. X-ray adaptive mirrors exhibit many advantages over the classical bendable mirrors, such as mechanics-free, figure local corrections, and good focusing properties. The piezoelectric bimorph mirrors have been used in astronomy to correct the wavefront distortions introduced by atmospheric turbulence in real time. The piezoelectric bimorph mirror was first introduced into the field of synchrotron radiation by European Synchrotron Radiation Facility (ESRF) in the 1990s for making an X-ray reflective mirror. Compared with astronomy community, synchrotron radiation community is not interested in high-speed wavefront correction, but looking for the ultimate precision of the surface shape of piezoelectric bimorph mirror. In the second part of this paper, the usual structure and working principle are briefly described. Piezoelectric bimorph mirrors are laminated structures consisting of two strips of an active material such as zirconate lead titanate (PZT) and two faceplates of a reflecting material such as silicon. A discrete or continuous control electrode is located between the interfaces of PZT-PZT, while two continuous ground electrodes are located between the interfaces of Si-PZT. The PZTs that are polarized normally to their surface, any voltage applied across the bimorph results in a different change of the lateral dimensions of two PZTs, thereby leading to a bending of the whole structure. The relationship between the curvature of the bending mirror and voltage is given. In the third part of this paper, the technical issues as well as the design concepts are discussed in detail. Several Si-PZT-PZT-Si bimorph mirrors are first fabricated and tested by ESRF. The dimensions of each of them are 150 mm in length, 4045 mm in width, and 1518 mm in thickness. PZT is selected as an active material because of its high coupling factor, high piezoelectric coefficient, and high Curie temperature. The faceplates need to be easy to polish such as silicon and silica. Owing to the symmetrical layered structure Si-PZT-PZT-Si, the mirror is less sensitive to temperature variations from the process of bonding and polishing. The bimorph mirrors are confirmed to be promising by experimental tests. As the state-of-art polishing technique, elastic emission machining (EEM) becomes available commercially, and diamond light source brings EEM into the bimorph mirror to achieve a novel adaptive X-ray mirror coupling adaptive zonal control with a super-smooth surface. This super-polished adaptive mirror becomes the first optics with a bendable ellipse with sub-nanometer figure error. Spring-8 fabricates an adaptive mirror with different structures, and two strips of PZTs are glued to the side faces of the mirror. This mirror shows a diffraction-limited performance. Finally, the wavefront measuring methods and control algorithm are introduced. Wavefront measuring devices used in the metrology cleanroom include long trace profiler, nanometer optics component measuring machine, and interferometer. At-wavelength measuring methods used on the beamline include pencil-beam method, phase retrieval method, X-ray speckle tracking technique, and Hartmann test. The wavefront control algorithm is aimed at obtaining the voltages applied according to the inverse of the interaction matrix.

Real-time observation of coherent acoustic phonons generated by an acoustically mismatched optoacoustic transducer using x-ray diffraction

The spectrum of laser-generated acoustic phonons in indium antimonide coated with a thin nickel film has been studied using time-resolved x-ray diffraction. Strain pulses that can be considered to be built up from coherent phonons were generated in the nickel film by absorption of short laser pulses. Acoustic reflections at the Ni–InSb interface leads to interference that strongly modifies the resulting phonon spectrum. The study was performed with high momentum transfer resolution together with high time resolution. This was achieved by using a third-generation synchrotron radiation source that provided a high-brightness beam and an ultrafast x-ray streak camera to obtain a temporal resolution of 10 ps. We also carried out simulations, using commercial finite element software packages and on-line dynamic diffraction tools. Using these tools, it is possible to calculate the time-resolved x-ray reflectivity from these complicated strain shapes. The acoustic pulses have a peak strain amplitude close to 1%, and we investigated the possibility to use this device as an x-ray switch. At a bright source optimized for hard x-ray generation, the low reflectivity may be an acceptable trade-off to obtain a pulse duration that is more than an order of magnitude shorter.

Revisit: High resolution charge density study of α-rhombohedral boron using third-generation SR data at SPring-8

Experimental charge density of α-rhombohedral boron (α-B12) by a Maximum entropy method (MEM) has been re-investigated using the high resolution powder diffraction data measured at third-generation synchrotron radiation (SR) source, SPring-8. The present MEM charge density has many discrepancies from the previous MEM charge densities reported by Fujimori et al. and Hosoi et al. The data-resolution dependence of the MEM charge density was investigated using the present data. We found that diffraction data with d > 0.4 Å resolution range were needed to reveal qualitative bonding nature of α-B12 at 100 K. The peculiar bonding natures, such as a bend B–B bond and a propeller-shaped bond, which were found in the previous studies have disappeared by using d > 0.4 Å data. The bonding nature of MEM charge density using the full data with d > 0.327 Å d-spacing range is well agreed with those of theoretical calculations. The present study suggests that resolution test is important for an accurate charge density study of boron related materials.

X선의 초고속 결정구조 측정법

무기단결정을 광 펄스로 여기 한 격자에서 광학이나 음향포논을 이용하여 광 여기 반도체가 서브피코초로 관측하고 있다. 다수의 회절 점으로 결정구조를 파악하는 것으로써 광 여기에 의한 분자결정 구조변화를 관측하는 것이 보고되고 있고 또한 반응이 진행되고 있는 중에 분자구조를 하나하나 영상으로 관측하는 것이 연구되고 있다. 단백질 분자구조의 시간에 따른 변화와 용액 중 분자의 광반응에 따른 구조변화를 파악하고 있는데 이것은 시스템에 따라 펨토 초에서 초 단위까지 다양하고 광범위하게 고도의 시간분해능으로 계측할 수 있는 X선 측정기술이다. We have surveyed on significant progress in recent developments of accelerator-based pulsed X-ray sources has offered the opportunity for time-resolved studies on fast structure dynamics on the nanometer scale. The required and currently available techniques for time resolved X-ray diffraction measurements using the third-generation synchrotron radiation sources are summarized. Ultrafast X-ray experimental techniques are discussed for femtosecond studies at future synchrotron radiation sources.

X-ray Raman scattering spectroscopy

For elements with low atomic number, or shallow absorption edges falling in the energy range below ~1 keV, x-ray absorption studies are often limited by surface sensitivity and the necessity of a vacuum environment, making bulk-sensitive measurements and for example studies of liquids difficult. An exciting alternative is provided by X-ray Raman scattering (XRS) spectroscopy. It is used to measure a photon-in-photon-out process, where a hard x-ray photon loses only part of its energy creating an excitation of an inner core electron. As such, it is the x-ray analogue of electron energy loss spectroscopy. The advantage of XRS is that the incident photon energy can be chosen freely and thus low-energy absorption edges can be studied with high-energy X-rays. Thus XRS is becoming increasingly popular since it allows for bulk-sensitive measurements of inner core spectra where the corresponding x-ray absorption threshold falls into the soft x-ray regime. This lifts all constraints on the sample environment inherent to soft x-ray studies, and offers access to bulk-sensitive information on solids, liquids and gases as well as systems in enclosed sample environments such as high-pressure cells. For example the microscopic structure of water within the supercritical regime has been recently studied using the oxygen K-edge excitation spectra measured by XRS, yielding new information on the hydrogen-bond network of water in extreme conditions [1]. Another important feature of XRS is that it allows for other than dipole transitions to be studied, thanks to an practically unlimited range of momentum transfer offered by hard x-rays. These higher order multipole excitations can yield novel information on the electronic structure, not accessible by many other spectroscopies [2]. The availability of XRS instruments at third-generation synchrotron radiation sources has made highly accurate XRS measurements possible. XRS can be even used as a contrast mechanism in three-dimensional X-ray imaging [3]. In this contribution, the capabilities of XRS and recent examples of novel studies allowed by it will be reviewed.

Probing the Self-Assembled Nanostructures of Functional Polymers with Synchrotron Grazing Incidence X-Ray Scattering

For advanced functional polymers such as biopolymers, biomimic polymers, brush polymers, star polymers, dendritic polymers, and block copolymers, information about their surface structures, morphologies, and atomic structures is essential for understanding their properties and investigating their potential applications. Grazing incidence X-ray scattering (GIXS) is established for the last 15 years as the most powerful, versatile, and nondestructive tool for determining these structural details when performed with the aid of an advanced third-generation synchrotron radiation source with high flux, high energy resolution, energy tunability, and small beam size. One particular merit of this technique is that GIXS data can be obtained facilely for material specimens of any size, type, or shape. However, GIXS data analysis requires an understanding of GIXS theory and of refraction and reflection effects, and for any given material specimen, the best methods for extracting the form factor and the structure factor from the data need to be established. GIXS theory is reviewed here from the perspective of practical GIXS measurements and quantitative data analysis. In addition, schemes are discussed for the detailed analysis of GIXS data for the various self-assembled nanostructures of functional homopolymers, brush, star, and dendritic polymers, and block copolymers. Moreover, enhancements to the GIXS technique are discussed that can significantly improve its structure analysis by using the new synchrotron radiation sources such as third-generation X-ray sources with picosecond pulses and partial coherence and fourth-generation X-ray laser sources with femtosecond pulses and full coherence.

X-ray harmonics rejection on third-generation synchrotron sources using compound refractive lenses.

A new method of harmonics rejection based on X-ray refractive optics has been proposed. Taking into account the fact that the focal distance of the refractive lens is energy-dependent, the use of an off-axis illumination of the lens immediately leads to spatial separation of the energy spectrum by focusing the fundamental harmonic at the focal point and suppressing the unfocused high-energy radiation with a screen absorber or slit. The experiment was performed at the ESRF ID06 beamline in the in-line geometry using an X-ray transfocator with compound refractive lenses. Using this technique the presence of the third harmonic has been reduced to 10(-3). In total, our method enabled suppression of all higher-order harmonics to five orders of magnitude using monochromator detuning. The method is well suited to third-generation synchrotron radiation sources and is very promising for the future ultimate storage rings.

At-wavelength Metrology of X-ray Optics at Diamond Light Source

Modern third-generation synchrotron radiation sources provide coherent and extremely bright X-ray beams, but the performance of the optics employed on the beamlines is critical for the X-rays' successful exploitation. The quality of the beam delivered to the sample is limited by the optics' imperfections and misalignment. Though the optics are accurately evaluated in metrology labs equipped with visible-light-based measuring instruments, such ex-situ characterizations do not allow perfect predictions of their beamline performance, since the mechanical and thermal strains imposed by beamline operation cannot be perfectly modelled. In-situ at-wavelength characterization is the natural way to overcome this limitation [1]. In-situ wavefront sensing performed at the optics' operating wavelength (“at-wavelength” metrology) can be used not only to optimize the performance of X-ray optics, but also to correct and minimize the collective distortions of upstream beamline optics (e.g., monochromator, windows, etc.). This issue has become even more critical with the increasing use of active optics on the beamlines on one hand, and with the desire to achieve diffraction-limited and coherence-preserved beams [2] on the other.

Profile measurement of concave spherical mirror and a flat mirror using a high-speed nanoprofiler

Ultraprecise aspheric mirrors that offer nanofocusing and high coherence are indispensable for developing third-generation synchrotron radiation and X-ray free-electron laser sources. In industry, the extreme ultraviolet (wavelength: 13.5 nm) lithography used for high-accuracy aspheric mirrors is a promising technology for fabricating semiconductor devices. In addition, ultraprecise mirrors with a radius of curvature of less than 10 mm are needed in many digital video instruments. We developed a new type of nanoprofiler that traces the normal vector of a mirror's surface. The principle of our measuring method is that the normal vector at each point on the surface is determined by making the incident light beam on the mirror surface and the reflected beam at that point coincide, using two sets of two pairs of goniometers and one linear stage. From the acquired normal vectors and their coordinates, the three-dimensional shape is calculated by a reconstruction algorithm. The characteristics of the measuring method are as follows: the profiler uses the straightness of laser light without using a reference surface. Surfaces of any shape can be measured, and there is no limit on the aperture size. We calibrated this nanoprofiler by considering the system error resulting from the assembly error and encoder scale error, and evaluated the performance at the nanometer scale. We suppressed the effect of random errors by maintaining the temperature in a constant-temperature room within ±0.01°C. We measured a concave spherical mirror with a radius of curvature of 400 mm and a flat mirror and compared the results with those obtained using a Fizeau interferometer. The profiles of the mirrors were consistent within the range of system errors.

Introduction: From a First-Generation Synchrotron Radiation to an X-ray Free Electron Laser

The fruitful and remarkable research results in materials science during the past more than ten years have been continuously obtained by the advent of synchrotron radiation (SR) sources, especially the third-generation SR source. This is easily understood by considering that the SR beams provide not only five to ten orders of magnitude brilliance more in the continuum vacuum ultraviolet and X-ray regions of the electromagnetic spectrum than conventional sources, but also natural collimation, high polarization, pulsed time structure and high stability. In this paper we present a brief history of SR sources, especially in Japan to know how the SR sources developed, and a view of the future research direction regarding the use of SR beams.

In Situ Time-Resolved SAXS Study of the Formation of Mesostructured Organically Modified Silica through Modeling of Micelles Evolution during Surfactant-Templated Self-Assembly

The mechanisms of formation of organically modified (phenyl, vinyl, and methyl) silica materials with cubic Pm3n and hexagonal p6m periodic mesostructures obtained in one step in the presence of the cetyltrimethylammonium bromide (CTA(+)B) surfactant are reported in this study. Understanding the way these complex materials form is difficult but undoubtedly necessary for controlling the material structure and its properties because of the combined presence of surface organic groups and large surface areas. Here, the mechanism of formation is clarified on the basis of the modeling of time-resolved in situ small angle X-ray scattering (SAXS) experiments, with a specific focus on the micelle evolution during material formation. Their fast self-assembly is followed for the first time with a quick temporal resolution of a few seconds using a third-generation synchrotron radiation source. To better understand the behavior of the complex organic-containing mesostructure, we perform a comparative study with the corresponding organo-free, isostructural materials obtained from three different surfactants (CTA(+), CTEA(+), and CTPA(+)) having a constant chain length (C(16)) and an increasing polar head volume (met-, et-, and prop-). Numerical modeling of SAXS data was crucial to highlighting a systematic sphere-to-rod micellar transition, otherwise undetected, before the formation of the 2D hexagonal phase in both organo-free and organo-containing systems. Then, two different pathways were found in the formation of the cubic Pm3n mesostructure: either an ordering transition from concentrated flocs of spherical micelles (from CTEA(+) or CTPA(+)) for pure TEOS systems or a structural transformation from an intermediate 2D hexagonal mesophase in organosilane systems (from CTA(+)). Combining the comparison between organo-free and organo-containing systems with numerical modeling, we find that the hexagonal-to-cubic phase transition in the organically modified materials seems to be strongly influenced not only by the obvious presence of the organic group but also by the quicker and more massive condensation kinetics of silicate oligomers on the CTA(+) micellar surface. Finally, quite unexpectedly, we find a wormlike-to-sphere micellar transition in the CTPA(+) system.

IR and X-ray time-resolved simultaneous experiments: an opportunity to investigate the dynamics of complex systems and non-equilibrium phenomena using third-generation synchrotron radiation sources

Third-generation storage rings are modern facilities working with high currents and designed to host powerful radiation sources, like undulators and wigglers, and to deliver high-brilliance beams to users. Many experiments at high spatial resolution, such as spectromicroscopy at the nanometre scale and with high temporal resolution to investigate kinetics down to the picosecond regime, are now possible. The next frontier is certainly the combination of different methods in a unique set-up with the ultimate available spatial and temporal resolutions. In the last decade much synchrotron-based research has exploited the advantage of complementary information provided by time-resolved X-ray techniques and optical methods in the UV/Vis and IR domains. New time-resolved and concurrent approaches are necessary to characterize complex systems where physical-chemical phenomena occur under the same experimental conditions, for example to detect kinetic intermediates via complementary but independent observations. In this contribution we present scientific cases from original works and literature reviews to support the proposed IR/X-ray simultaneous approach, with both probes exploiting synchrotron radiation sources. In addition, simple experimental layouts that may take advantage of the high brilliance and the wide spectral distribution of the synchrotron radiation emission will be given for specific researches or applications to investigate dynamic processes and non-equilibrium phenomena occurring in many condensed matter and biological systems, of great interest for both fundamental research and technological applications.

Computer analysis of two-dimensional images in the Zernike phase contrast method for hard X rays

The problems of the numerical simulation of two-dimensional images in the Zernike phase contrast method in hard X rays are analyzed. Calculations are performed for experimental conditions typical of third-generation synchrotron radiation sources (ESRF, APS, Spring-8, etc.). Schemes are considered where the focusing elements are a refracting lens and a zone plate and the phase-shifting element is situated at the point of the source image. It is shown that the refracting lens allows better resolution than the zone plate. A technique similar to ptychography can be successfully applied to improve the quality of the images obtained by the Zernike phase contrast method.

Quantitative performance measurements of bent crystal Laue analyzers for X-ray fluorescence spectroscopy

Third-generation synchrotron radiation sources pose difficult challenges for energy-dispersive detectors for XAFS because of their count rate limitations. One solution to this problem is the bent crystal Laue analyzer (BCLA), which removes most of the undesired scatter and fluorescence before it reaches the detector, effectively eliminating detector saturation due to background. In this paper experimental measurements of BCLA performance in conjunction with a 13-element germanium detector, and a quantitative analysis of the signal-to-noise improvement of BCLAs are presented. The performance of BCLAs are compared with filters and slits.

The high-resolution diffraction beamline P08 at PETRA III

The new third-generation synchrotron radiation source PETRA III located at the Deutsches Elektronen-Synchrotron DESY in Hamburg, Germany, has been operational since the second half of 2009. PETRA III is designed to deliver hard X-ray beams with very high brilliance. As one of the first beamlines of PETRA III the high-resolution diffraction beamline P08 is fully operational. P08 is specialized in X-ray scattering and diffraction experiments on solids and liquids where extreme high resolution in reciprocal space is required. The resolving power results in the high-quality PETRA III beam and unique optical elements such as a large-offset monochromator and beryllium lens changers. A high-precision six-circle diffractometer for solid samples and a specially designed liquid diffractometer are installed in the experimental hutch. Regular users have been accepted since summer 2010.