scholarly journals Tracking the Local Structure Change during the Photoabsorption Processes of Photocatalysts by the Ultrafast Pump-Probe XAFS Method

2020 ◽  
Vol 10 (21) ◽  
pp. 7818
Author(s):  
Yohei Uemura ◽  
Toshihiko Yokoyama ◽  
Tetsuo Katayama ◽  
Shunsuke Nozawa ◽  
Kiyotaka Asakura
Keyword(s):  
Structural Change ◽  
Free Electron ◽  
Structure Change ◽  
Ground State Structure ◽  
X Rays ◽  
Geometrical Structures ◽  
Band Theory ◽  
Pump Probe ◽  
X Ray ◽  
Wide Range

The birth of synchrotron radiation (SR) facilities and X-ray free electron lasers (XFELs) has led to the development of new characterization tools that use X-rays and opened frontiers in science and technology. Ultrafast X-ray absorption fine structure (XAFS) spectroscopy for photocatalysts is one such significant research technique. Although carrier behavior in photocatalysts has been discussed in terms of the band theory and their energy levels in reciprocal space (k-space) based on optical spectroscopic results, it has rarely been discussed where photocarriers are located in real-space (r-space) based on direct observation of the excited states. XAFS provides information on the local electronic and geometrical structures around an X-ray-absorbing atom and can address photocarrier dynamics in the r-space observed from the X-ray-absorbing atom. In this article, we discuss the time dependent structure change of tungsten trioxide (WO3) and bismuth vanadate (BiVO4) photocatalysts studied by the ultrafast pump-probe XAFS method in the femtosecond to nanosecond time scale with the Photon Factory Advanced Ring (PF-AR) and the SPring-8 Angstrom Compact free-electron LAser (SACLA). WO3 shows a femtosecond decay process of photoexcited electrons followed by a structural change to a metastable state with a hundred picosecond speed, which is relaxed to the ground-state structure with a nanosecond time constant. The Bi L3 edge of BiVO4 shows little contribution of the Bi 6s electron to the photoabsorption process; however, it is sensitive to the structural change induced by the photoexcited electron. Time-resolved XAFS measurements in a wide range time domain and with varied wavelengths of the excitation pump laser facilitate understanding of the overall details regarding the photocarrier dynamics that have a significant influence on the photocatalytic performance.

scholarly journals Double chirp-taper x-ray free-electron laser for attosecond pump-probe experiments

2019 ◽  
Vol 22 (5) ◽  
Author(s):  
Zhen Zhang ◽  
Joseph Duris ◽  
James P. MacArthur ◽  
Zhirong Huang ◽  
Agostino Marinelli
Keyword(s):  
Free Electron ◽  
Free Electron Laser ◽  
Pump Probe ◽  
X Ray

scholarly journals The XXL Survey

2018 ◽  
Vol 620 ◽  
pp. A18 ◽  
Author(s):  
C. H. A. Logan ◽  
B. J. Maughan ◽  
M. N. Bremer ◽  
P. Giles ◽  
M. Birkinshaw ◽  
...  
Keyword(s):  
Angular Resolution ◽  
False Positive Rate ◽  
High Sensitivity ◽  
Point Sources ◽  
Selection Function ◽  
X Rays ◽  
Cluster Emission ◽  
X Ray ◽  
Wide Range ◽  
Function Modelling

Context. The XMM-XXL survey has used observations from the XMM-Newton observatory to detect clusters of galaxies over a wide range in mass and redshift. The moderate PSF (FWHM ~ 6″ on-axis) of XMM-Newton means that point sources within or projected onto a cluster may not be separated from the cluster emission, leading to enhanced luminosities and affecting the selection function of the cluster survey. Aims. We present the results of short Chandra observations of 21 galaxy clusters and cluster candidates at redshifts z > 1 detected in the XMM-XXL survey in X-rays or selected in the optical and infra-red. Methods. With the superior angular resolution of Chandra, we investigate whether there are any point sources within the cluster region that were not detected by the XMM-XXL analysis pipeline, and whether any point sources were misclassified as distant clusters. Results. Of the 14 X-ray selected clusters, 9 are free from significant point source contamination, either having no previously unresolved sources detected by Chandra or with less than about 10% of the reported XXL cluster flux being resolved into point sources. Of the other five sources, one is significantly contaminated by previously unresolved AGN, and four appear to be AGN misclassified as clusters. All but one of these cases are in the subset of less secure X-ray selected cluster detections and the false positive rate is consistent with that expected from the XXL selection function modelling. We also considered a further seven optically selected cluster candidates associated with faint XXL sources that were not classed as clusters. Of these, three were shown to be AGN by Chandra, one is a cluster whose XXL survey flux was highly contaminated by unresolved AGN, while three appear to be uncontaminated clusters. By decontaminating and vetting these distant clusters, we provide a pure sample of clusters at redshift z > 1 for deeper follow-up observations, and demonstrate the utility of using Chandra snapshots to test for AGN in surveys with high sensitivity but poor angular resolution.

A multi-length-scale USAXS/SAXS facility: 10–50 keV small-angle X-ray scattering instrument

2013 ◽  
Vol 46 (5) ◽  
pp. 1508-1512 ◽  
Author(s):  
Byron Freelon ◽  
Kamlesh Suthar ◽  
Jan Ilavsky
Keyword(s):  
Small Angle ◽  
Soft Matter ◽  
High Energy ◽  
X Rays ◽  
X Ray ◽  
X Ray Scattering ◽  
Wide Range ◽  
And Performance ◽  
New Facility ◽  
Ray Scattering

Coupling small-angle X-ray scattering (SAXS) and ultra-small-angle X-ray scattering (USAXS) provides a powerful system of techniques for determining the structural organization of nanostructured materials that exhibit a wide range of characteristic length scales. A new facility that combines high-energy (HE) SAXS and USAXS has been developed at the Advanced Photon Source (APS). The application of X-rays across a range of energies, from 10 to 50 keV, offers opportunities to probe structural behavior at the nano- and microscale. An X-ray setup that can characterize both soft matter or hard matter and high-Zsamples in the solid or solution forms is described. Recent upgrades to the Sector 15ID beamline allow an extension of the X-ray energy range and improved beam intensity. The function and performance of the dedicated USAXS/HE-SAXS ChemMatCARS-APS facility is described.

scholarly journals Stellar Winds in Massive X-ray Binaries

2016 ◽  
Vol 12 (S329) ◽  
pp. 355-358
Author(s):  
Peter Kretschmar ◽  
Silvia Martínez-Núñez ◽  
Enrico Bozzo ◽  
Lidia M. Oskinova ◽  
Joachim Puls ◽  
...  
Keyword(s):  
Compact Object ◽  
High Mass ◽  
Stellar Winds ◽  
X Rays ◽  
X Ray ◽  
Current State ◽  
Wide Range ◽  
Strong Winds ◽  
The One ◽  
X Ray Binaries

AbstractStrong winds from massive stars are a topic of interest to a wide range of astrophysical fields. In High-Mass X-ray Binaries the presence of an accreting compact object on the one side allows to infer wind parameters from studies of the varying properties of the emitted X-rays; but on the other side the accretor’s gravity and ionizing radiation can strongly influence the wind flow. Based on a collaborative effort of astronomers both from the stellar wind and the X-ray community, this presentation attempts to review our current state of knowledge and indicate avenues for future progress.

scholarly journals Methods development for diffraction and spectroscopy studies of metalloenzymes at X-ray free-electron lasers

2014 ◽  
Vol 369 (1647) ◽  
pp. 20130590 ◽  
Author(s):  
Jan Kern ◽  
Johan Hattne ◽  
Rosalie Tran ◽  
Roberto Alonso-Mori ◽  
Hartawan Laksmono ◽  
...  
Keyword(s):  
Free Electron ◽  
Water Oxidation ◽  
Spectroscopic Studies ◽  
Free Electron Lasers ◽  
Software Suite ◽  
X Ray ◽  
Methods Development ◽  
Wide Range ◽  
Linac Coherent Light Source ◽  
Spectroscopy Studies

X-ray free-electron lasers (XFELs) open up new possibilities for X-ray crystallographic and spectroscopic studies of radiation-sensitive biological samples under close to physiological conditions. To facilitate these new X-ray sources, tailored experimental methods and data-processing protocols have to be developed. The highly radiation-sensitive photosystem II (PSII) protein complex is a prime target for XFEL experiments aiming to study the mechanism of light-induced water oxidation taking place at a Mn cluster in this complex. We developed a set of tools for the study of PSII at XFELs, including a new liquid jet based on electrofocusing, an energy dispersive von Hamos X-ray emission spectrometer for the hard X-ray range and a high-throughput soft X-ray spectrometer based on a reflection zone plate. While our immediate focus is on PSII, the methods we describe here are applicable to a wide range of metalloenzymes. These experimental developments were complemented by a new software suite, cctbx.xfel . This software suite allows for near-real-time monitoring of the experimental parameters and detector signals and the detailed analysis of the diffraction and spectroscopy data collected by us at the Linac Coherent Light Source, taking into account the specific characteristics of data measured at an XFEL.

scholarly journals Nanofocusing Optics for an X-Ray Free-Electron Laser Generating an Extreme Intensity of 100 EW/cm2 Using Total Reflection Mirrors

2020 ◽  
Vol 10 (7) ◽  
pp. 2611
Author(s):  
Hirokatsu Yumoto ◽  
Yuichi Inubushi ◽  
Taito Osaka ◽  
Ichiro Inoue ◽  
Takahisa Koyama ◽  
...  
Keyword(s):  
Photon Energy ◽  
Pulse Energy ◽  
Free Electron ◽  
Free Electron Laser ◽  
Total Reflection ◽  
Experimental Chamber ◽  
X Rays ◽  
X Ray ◽  
Set Up ◽  
Focused Beam

A nanofocusing optical system—referred to as 100 exa—for an X-ray free-electron laser (XFEL) was developed to generate an extremely high intensity of 100 EW/cm2 (1020 W/cm2) using total reflection mirrors. The system is based on Kirkpatrick-Baez geometry, with 250-mm-long elliptically figured mirrors optimized for the SPring-8 Angstrom Compact Free-Electron Laser (SACLA) XFEL facility. The nano-precision surface employed is coated with rhodium and offers a high reflectivity of 80%, with a photon energy of up to 12 keV, under total reflection conditions. Incident X-rays on the optics are reflected with a large spatial acceptance of over 900 μm. The focused beam is 210 nm × 120 nm (full width at half maximum) and was evaluated at a photon energy of 10 keV. The optics developed for 100 exa efficiently achieved an intensity of 1 × 1020 W/cm2 with a pulse duration of 7 fs and a pulse energy of 150 μJ (25% of the pulse energy generated at the light source). The experimental chamber, which can provide different stage arrangements and sample conditions, including vacuum environments and atmospheric-pressure helium, was set up with the focusing optics to meet the experimental requirements.

scholarly journals High Repetition Rate and Coherent Free-Electron Laser in the X-Rays Range Tailored for Linear Spectroscopy

Instruments ◽  
2019 ◽  
Vol 3 (3) ◽  
pp. 47 ◽  
Author(s):  
Vittoria Petrillo ◽  
Michele Opromolla ◽  
Alberto Bacci ◽  
Illya Drebot ◽  
Giacomo Ghiringhelli ◽  
...  
Keyword(s):  
Free Electron ◽  
Repetition Rate ◽  
Free Electron Laser ◽  
Extreme Ultraviolet ◽  
High Harmonic ◽  
High Repetition Rate ◽  
X Rays ◽  
Regenerative Amplifier ◽  
X Ray ◽  
High Repetition

Fine time-resolved analysis of matter—i.e., spectroscopy and photon scattering—in the linear response regime requires fs-scale pulsed, high repetition rate, fully coherent X-ray sources. A seeded Free Electron Laser (FEL) driven by a Linac based on Super Conducting cavities, generating 10 8 – 10 10 coherent photons at 2–5 keV with 0.2–1 MHz of repetition rate, can address this need. Three different seeding schemes, reaching the X-ray range, are described hereafter. The first two are multi-stage cascades upshifting the radiation frequency by a factor of 10–30 starting from a seed represented by a coherent flash of extreme ultraviolet light. This radiation can be provided either by the High Harmonic Generation of an optical laser or by an FEL Oscillator operating at 12–14 nm. The third scheme is a regenerative amplifier working with X-ray mirrors. The whole chain of the X-ray generation is here described by means of start-to-end simulations.

scholarly journals A comparison of the radiosensitisation ability of 22 different element metal oxide nanoparticles using clinical megavoltage X-rays

2019 ◽  
Vol 10 (1) ◽  
Author(s):  
Alexandra Guerreiro ◽  
Nicholas Chatterton ◽  
Eleanor M. Crabb ◽  
Jon P. Golding
Keyword(s):  
Dna Damage ◽  
Metal Oxide ◽  
Hydroxyl Radical ◽  
Singlet Oxygen ◽  
Hydroxyl Radicals ◽  
Metal Oxide Nanoparticles ◽  
Oxide Nanoparticles ◽  
X Rays ◽  
X Ray ◽  
Wide Range

Abstract Background A wide range of nanoparticles (NPs), composed of different elements and their compounds, are being developed by several groups as possible radiosensitisers, with some already in clinical trials. However, no systematic experimental survey of the clinical X-ray radiosensitising potential of different element nanoparticles has been made. Here, we directly compare the irradiation-induced (10 Gy of 6-MV X-ray photon) production of hydroxyl radicals, superoxide anion radicals and singlet oxygen in aqueous solutions of the following metal oxide nanoparticles: Al2O3, SiO2, Sc2O3, TiO2, V2O5, Cr2O3, MnO2, Fe3O4, CoO, NiO, CuO, ZnO, ZrO2, MoO3, Nd2O3, Sm2O3, Eu2O3, Gd2O3, Tb4O7, Dy2O3, Er2O3 and HfO2. We also examine DNA damage due to these NPs in unirradiated and irradiated conditions. Results Without any X-rays, several NPs produced more radicals than water alone. Thus, V2O5 NPs produced around 5-times more hydroxyl radicals and superoxide radicals. MnO2 NPs produced around 10-times more superoxide anions and Tb4O7 produced around 3-times more singlet oxygen. Lanthanides produce fewer hydroxyl radicals than water. Following irradiation, V2O5 NPs produced nearly 10-times more hydroxyl radicals than water. Changes in radical concentrations were determined by subtracting unirradiated values from irradiated values. These were then compared with irradiation-induced changes in water only. Irradiation-specific increases in hydroxyl radical were seen with most NPs, but these were only significantly above the values of water for V2O5, while the Lanthanides showed irradiation-specific decreases in hydroxyl radical, compared to water. Only TiO2 showed a trend of irradiation-specific increase in superoxides, while V2O5, MnO2, CoO, CuO, MoO3 and Tb4O7 all demonstrated significant irradiation-specific decreases in superoxide, compared to water. No irradiation-specific increases in singlet oxygen were seen, but V2O5, NiO, CuO, MoO3 and the lanthanides demonstrated irradiation-specific decreases in singlet oxygen, compared to water. MoO3 and CuO produced DNA damage in the absence of radiation, while the highest irradiation-specific DNA damage was observed with CuO. In contrast, MnO2, Fe3O4 and CoO were slightly protective against irradiation-induced DNA damage. Conclusions Beyond identifying promising metal oxide NP radiosensitisers and radioprotectors, our broad comparisons reveal unexpected differences that suggest the surface chemistry of NP radiosensitisers is an important criterion for their success.

scholarly journals Demonstration of Transmission Mode Soft X-ray NEXAFS Using Third- and Fifth-Order Harmonics of FEL Radiation at SACLA BL1

2020 ◽  
Vol 10 (21) ◽  
pp. 7852
Author(s):  
Hiroshi Iwayama ◽  
Masanari Nagasaka ◽  
Ichiro Inoue ◽  
Shigeki Owada ◽  
Makina Yabashi ◽  
...  
Keyword(s):  
Fine Structure ◽  
Free Electron ◽  
Free Electron Laser ◽  
Transmission Mode ◽  
Pump Probe ◽  
X Ray ◽  
The Third ◽  
Nexafs Spectroscopy ◽  
Fifth Order ◽  
X Ray Absorption

We demonstrate the applicability of third- and fifth-order harmonics of free-electron laser (FEL) radiation for soft X-ray absorption spectroscopy in the transmission mode at SACLA BL1, which covers a photon energy range of 20 to 150 eV in the fundamental FEL radiation. By using the third- and fifth-order harmonics of the FEL radiation, we successfully recorded near-edge X-ray absorption fine structure (NEXAFS) spectra for Ar 2p core ionization and CO2 C 1s and O 1s core ionizations. Our results show that the utilization of third- and fifth-order harmonics can significantly extend the available photon energies for NEXAFS spectroscopy using an FEL and opens the door to femtosecond pump-probe NEXAFS using a soft X-ray FEL.

scholarly journals X-Ray Free-Electron Lasers for the Structure and Dynamics of Macromolecules

2019 ◽  
Vol 88 (1) ◽  
pp. 35-58 ◽  
Author(s):  
Henry N. Chapman
Keyword(s):  
Free Electron ◽  
Conformational Dynamics ◽  
Cryogenic Cooling ◽  
X Rays ◽  
Free Electron Lasers ◽  
X Ray ◽  
Virus Particles ◽  
Structure And Dynamics ◽  
Small Crystals ◽  
Serial Crystallography

X-ray free-electron lasers provide femtosecond-duration pulses of hard X-rays with a peak brightness approximately one billion times greater than is available at synchrotron radiation facilities. One motivation for the development of such X-ray sources was the proposal to obtain structures of macromolecules, macromolecular complexes, and virus particles, without the need for crystallization, through diffraction measurements of single noncrystalline objects. Initial explorations of this idea and of outrunning radiation damage with femtosecond pulses led to the development of serial crystallography and the ability to obtain high-resolution structures of small crystals without the need for cryogenic cooling. This technique allows the understanding of conformational dynamics and enzymatics and the resolution of intermediate states in reactions over timescales of 100 fs to minutes. The promise of more photons per atom recorded in a diffraction pattern than electrons per atom contributing to an electron micrograph may enable diffraction measurements of single molecules, although challenges remain.

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