Accelerator Laboratory Research Articles

Hard X-ray single-shot spectrometer of PAL-XFEL.

A transmissive single-shot spectrometer has been developed to monitor shot-to-shot spectral structures in the hard X-ray beamline of the Pohang Accelerator Laboratory X-ray Free Electron Laser (PAL-XFEL). The established spectrometer comprises 10 µm-thick Si crystals bent to a radius of curvature of 100 mm. Depending on the photon energy range, either the Si (111) or Si (110) crystal can be selected for spectral analysis. Especially in the energy range 4.5-17 keV, the spectrometer is designed to cover a spectral range wider than the full free-electron laser bandwidth and to guarantee a high resolution sufficient for resolving each spectral spike. This paper presents the design specifications, instruments and performance of this spectrometer, which has also been applied to demonstrate the spectral properties of various XFEL sources, such as self-amplified spontaneous emission, monochromatic and seeded beams.

γ-Ray spectroscopy above the 9+ isomeric state in the N = Z nucleus 66As

Excited states above the 9+ isomer in the odd-odd N = Z nucleus 66As were studied by employing the 40Ca(28Si, pn) fusion-evaporation reaction at the Accelerator Laboratory of the University of Jyväskylä, Finland. A key method in this study was the use of conversion electrons emitted in the de-excitation of the isomeric state in 66As as a tag for prompt γ rays. Several new states have been added to the 66As level scheme, which was extended up to a tentative spin of 23ħ. The previously reported even-spin yrast band has been reassigned to have odd spin values. The odd-spin states above the 9+ isomer are compared with shell-model calculations using the jj44b and JUN45 interactions. Additionally, the recoil-β tagging efficiency of the recently developed scintillator detector named Tuike has been determined experimentally for the first time.

Particle induced x-ray emission (pixe) assisted technique in the evaluation of potential ecological risks of heavy metals in surface sediments of Oba-Ile River, Ifelodun Local Government Area, Osun-State, Nigeria

The seasonal evaluation of trace elements in the surface sediments collected from Oba-Ile River, using Particle Induced X-Ray Emission (PIXE) Spectroscopy had been carried out. This was done so as to provide information about the pollution status of the river during the rainy and dry seasons. The samples were subjected to trace metal profiling using a 2.5 Mev proton available at the Ion Beam Analysis (IBA)/accelerator laboratory, Centre for Energy Research and Development (CERD), Obafemi Awolowo University, Ile-Ife. The facility is centered on a NEC 5SDH 1.7 MV Pelletron accelerator, equipped to provide proton and helium ions. A multi-elemental estuarine sediments referenced material (SRM 1646a purchased from NIST) was used for the determination of H-value which was subsequently used for analyzing the samples and assured the accuracy of the experimental procedure. The order of abundance of the 16 elements identified was Si > Fe >Al >K > Ca >Ti > Na > Mg > Zr > Mn > Sr > V > Cr > Zn > Pb > Cu. The contamination factor indicated that the metals presented a low contamination factor (LCf) to moderate contamination factor (MCf) except for Fe and Zr which presented a considerable contamination (CCf) and a very high contamination factor (VHCf) respectively. Other contamination indices indicated that Fe had either a moderate enrichment (ME) factor or a significant enrichment (SE) factor, thereby suggesting that Oba-Ile River sediment was particularly enriched in Fe

Fluorine and Nitrogen Doped Fe-Based Non-Precious Metal Catalyst for Highly Efficient Catalytic Oxygen Reduction Reaction in Alkaline Electrolyte

Anion exchange membrane fuel cells (AEMFCs) attract much attention since they play a crucial role in the hydrogen economy. The oxygen reduction reaction (ORR) at the cathode is a fundamental reaction in electrochemical energy conversion systems like AEMFCs. However, the kinetics of the ORR are sluggish and the precious metal catalysts such as Pt which are highly efficient for the ORR are scarce and costly. Owing to their disadvantages, it is required to replace the precious metal catalysts with abundant non-precious metal catalysts.In the past decade, the transition metal nitrogen carbon catalysts (M-N-C) have been accentuated as possible alternatives to Pt catalysts due to their wide applicability to electrochemical catalysis and high ORR performance in alkaline media [1, 2]. Fe is generally known as the most efficient transition metal for the ORR [3, 4]. However, the ORR activity of Fe-N-C catalysts is not competitive with that of Ptcatalysts. To boost the activity and performance of theFe-N-C catalyst, doping additional heteroatoms (such as B, S, P, and F) to the Fe–N–C catalysts is widely investigated since it is a simple and practical strategy.In this work, we synthesize Fe-N-F-C catalysts using chelating agents like ethylene diamine and ethylenediamine (EDA) and 1,1,1,5,5,5-hexafluoroacetylacetone (HFAc) as the N and F precursors, respectively. The annealing temperature and doped heteroatoms were systematically designed to arrange control samples to elucidate their synergistic effects on the ORR activity. We used high-resolution transmission electron microscopy (HR-TEM), X-ray diffraction (XRD), Raman spectroscopy, Inductively coupled plasma-optical emission spectrometry (ICP-OES), X-ray photoelectron spectroscopy (XPS), X-ray absorption near edge structure (XANES) and extended X-ray absorption fine structure (EXAFS) using the 1D-XRS KIST-PAL beamline of the PLS-II light source at the Pohang Accelerator Laboratory as well as a rotating ring disk electrode (RRDE) system.Well-dispersed uniform iron carbide particles were detected in Fe@NFC700 by HR-TEM. Among the catalysts, the highest amount of heteroatom functional groups (i.e. semi-ionic C–F bonds and Fe–Nx) that expedite the ORR activity were observed in Fe@NFC700. In addition, Fe@NFC700 exhibited higher contents of the Fe–Nx, pyridinic-N, and graphitic-N than Fe@NC, which indicates that F doping influences the formation of the N functional groups. As a result, Fe@NFC700 showed a high onset potential (0.981 V) and a small Tafel slope (79.11 mV dec‒1) compared to the catalysts synthesized at different annealing temperatures. The F-doped Fe–N–C system is a highly potential candidate for electrochemical energy applications such as AEMFCs and metal-air batteries.This work was supported by the National Research Foundation of Korea (NRF) grant funded by the Korea government (MSIT) (No. 2020R1C1C1004206).

High-resolution laser spectroscopy of singly charged natural uranium isotopes

High-resolution collinear laser spectroscopy has been performed on singly charged ions of 234,235,238\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$^{234,235,238}$$\\end{document}U at the IGISOL facility of the Accelerator Laboratory, University of Jyväskylä, in Finland. Ten ionic transitions from the 4I9/2\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$^{4}\\hbox {I}_{9/2}$$\\end{document} and 6L11/2\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$^{6}\\hbox {L}_{11/2}$$\\end{document} ground and first excited states were measured in the 300 nm wavelength range, improving the precision of the hyperfine parameters of the lower states in addition to providing newly measured values for the upper levels. Isotope shifts of the analyzed transitions are also reported for 234,235\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$^{234,235}$$\\end{document}U with respect to 238\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$^{238}$$\\end{document}U.

Structural evolution of liquid silicates under conditions in Super-Earth interiors

Molten silicates at depth are crucial for planetary evolution, yet their local structure and physical properties under extreme conditions remain elusive due to experimental challenges. In this study, we utilize in situ X-ray diffraction (XRD) at the Matter in Extreme Conditions (MEC) end-station of the Linear Coherent Linac Source (LCLS) at SLAC National Accelerator Laboratory to investigate liquid silicates. Using an ultrabright X-ray source and a high-power optical laser, we probed the local atomic arrangement of shock-compressed liquid (Mg,Fe)SiO3 with varying Fe content, at pressures from 81(9) to 385(40) GPa. We compared these findings to ab initio molecular dynamics simulations under similar conditions. Results indicate continuous densification of the O-O and Mg-Si networks beyond Earth’s interior pressure range, potentially altering melt properties at extreme conditions. This could have significant implications for early planetary evolution, leading to notable differences in differentiation processes between smaller rocky planets, such as Earth and Venus, and super-Earths, which are exoplanets with masses nearly three times that of Earth.

Quantitative x-ray scattering of free molecules

Abstract Advances in X-ray free electron lasers have made ultrafast scattering a powerful method for investigating molecular reaction kinetics and dynamics. Accurate measurement of the ground-state, static scattering signals of the reacting molecules is pivotal for these pump-probe X-ray scattering experiments as they are the cornerstone for interpreting the observed structural dynamics. This article presents a data calibration procedure, designed for gas-phase X-ray scattering experiments conducted at the Linac Coherent Light Source X-ray Free-Electron Laser at SLAC National Accelerator Laboratory, that makes it possible to derive a quantitative dependence of the scattering signal on the scattering vector. A self-calibration algorithm that optimizes the detector position without reference to a computed pattern is introduced. Angle-of-scattering corrections that account for several small experimental non-idealities are reported. Their implementation leads to near quantitative agreement with theoretical scattering patterns calculated with ab-initio methods as illustrated for two X-ray photon energies and several molecular test systems.

Gain stability of Hamamatsu R5912-MOD photomultipliers at low temperature

The Photon Detection System (PDS) is a crucial component of the ICARUS detector in the Short Baseline Neutrino (SBN) Program at Fermi National Accelerator Laboratory (FNAL). It consists of 360 PhotoMultiplier Tubes (PMTs) 8” Hamamatsu R5912-MOD and, since June 2020, it has been operating at the liquid Argon cryogenic temperature. During these years, the PMTs have shown gain losses as an aging effect. Using a climatic chamber at the INFN Sezione di Catania, we confirmed a stable gain for a single PMT 8” Hamamatsu R5912-MOD when operated at room temperature, and a persistent gain loss at temperatures around -70 °C, although this temperature is rather higher than that of the liquid Argon.

Decay of a microsecond seniority 3 isomeric state in Hf155

Excited states in the neutron-deficient nuclide Hf155 have been investigated in experiments performed at the Accelerator Laboratory of the University of Jyväskylä. The Hf155 nuclei were produced in fusion-evaporation reactions induced by beams of 295 and 315 MeV Ni58 ions bombarding an isotopically enriched Pd102 target and separated using the recoil mass separator MARA. An isomeric state having a half-life of 510(30) ns was discovered and is interpreted as a seniority υ=3, (πh11/22⊗νf7/2)27/2− configuration. The γ-ray transitions emitted in the deexcitation of the isomeric state to the ground state were identified and a level scheme was constructed, from which the excitation energy of the isomer was determined to be 2581.5(10) keV. A B(E2) value of 0.45(3) W.u. was deduced for the 105.4 keV transition depopulating the isomeric state. The deduced level scheme and B(E2) value are compared with systematics and shell-model calculations. Published by the American Physical Society 2024

A high throughput facility for the RF characterisation Of planar superconducting thin films

Abstract Accelerator laboratories worldwide are researching copper radio frequency (RF) cavities coated with superconducting thin films to exceed the limits of bulk niobium. The development and RF testing of thin films on small planar samples is vital before cavity depositions. A team at Daresbury Laboratory have developed a cost-effective facility using a novel 7.8 GHz Choke Cavity for the RF characterisation of planar samples. RF chokes ensure that no electrical contact is required between the sample and the cavity. The main advantages are: a simple sample design (90 − 130 mm diameter disk with no sample-cavity welding) and easy operation using a LHe-free cryostat. This enables high sample throughput, with up to 3 sample tests per week, making the facility suitable for quick, systematic scanning of deposition parameters. With the sample thermally and physically isolated from the test cavity, it is possible to measure the average surface resistance, R s, directly using an RF-DC compensation method. Facility commissioning has been performed with bulk and thin film niobium samples. These tests have demonstrated the ability to measure R s at temperatures in the range 4 − 20 K and sample peak magnetic fields up to 3 mT. The minimum resolvable R s is 0.5 μΩ with typical uncertainties of 9 − 15%. The design, operation and commissioning of this facility is reported in this paper.

Real-time study of radiation damage in monocrystalline diamond sensors

Being an excellent radiation hard material, diamond is preferred as an ionizing radiation sensor in radiation harsh environments. In this study, radiation damage from a beam of 67.5 MeV protons at the Crocker Nuclear Laboratory on the campus of the University of California, Davis, was used to determine exposure lifetime in detectors made from a thinned (∼ 40 μm) monocrystalline CVD (chemical vapor deposition) diamond substrate. The sensor response was sampled in real time as the sensor was exposed to a total fluence of ∼ 4×1016 / cm2, yielding an overall damage constant of k = (3.3 ± 0.3) × 10-18 cm2 / p-μm. Damage levels were later confirmed using a non-destructive x-ray technique at the LINAC Coherent Light Source (LCLS) at the SLAC National Accelerator Laboratory. Results are presented on the real-time degradation of the charge collection efficiency as a function of proton fluence.

Search by the SENSEI Experiment for Millicharged Particles Produced in the NuMI Beam.

Millicharged particles appear in several extensions of the standard model, but have not yet been detected. These hypothetical particles could be produced by an intense proton beam striking a fixed target. We use data collected in 2020 by the SENSEI experiment in the MINOS cavern at the Fermi National Accelerator Laboratory to search for ultrarelativistic millicharged particles produced in collisions of protons in the NuMI beam with a fixed graphite target. The absence of any ionization events with 3 to 6 electrons in the SENSEI data allow us to place world-leading constraints on millicharged particles for masses between 30 to 380MeV. This work also demonstrates the potential of utilizing low-threshold detectors to investigate new particles in beam-dump experiments, and motivates a future experiment designed specifically for this purpose.

(Invited) Innovating Sustainable, Cost-Effective, and Durable Redox Flow Battery Membranes

In the quest to integrate renewable energy sources like solar and wind into the electric grid efficiently, the development of long-duration energy storage (LDES) systems is paramount. The U.S. Department of Energy's Long Duration Storage Shot initiative is at the forefront of this endeavor, aiming to reduce the costs of grid-scale energy storage by 90% for systems with over 10 hours of operation. A key player in this mission is the non-aqueous redox flow battery (RFB), known for its use of earth-abundant materials and potential to meet these cost-reduction goals. However, the commercial viability of RFBs hinges on the development of high-performance, cost-effective membranes, which are crucial for their functionality and affordability. These membranes' ionic conductivity is vital for the power density of RFBs, while their ion selectivity and solvent uptake greatly influence the batteries' cycle life.Our team has made groundbreaking advancements in membrane technology for non-aqueous flow batteries. We've addressed the challenge of balancing ionic conductivity with mechanical strength in polymer electrolytes. Our findings reveal that enhanced solvent uptake while boosting membrane ionic conductivity, can compromise mechanical integrity. To counter this, we've employed two strategies: selective plasticization of the ion-conductive block in block copolymers and reinforcing the membrane's mechanical strength through hydrogen and ionic bonds with an inorganic scaffold. Significantly, we've also reduced the crossover of redox-active species in our membrane designs, notably decreasing polysulfide species crossover in a Na metal – polysulfide hybrid flow battery. This has led to improved capacity retention, Coulombic efficiency, and extended cycle life compared to traditional porous membranes.Our latest innovations include the development of hydrocarbon single-ion conductors, demonstrating enhanced conductivity and stability. We've also introduced crosslinking chemistry to control solvent uptake more effectively, thus improving ionic conductivity while preserving mechanical strength. Lastly, our pioneering tape casting method for producing ceramic-polymer composite membranes represents a major leap in scalable membrane production, paving the way for the practical application of non-aqueous redox flow batteries in long-duration energy storage. Acknowledgment This research was conducted at Oak Ridge National Laboratory, managed by UT Battelle, LLC, for the U.S. Department of Energy (DOE) and is sponsored by the U.S. Department of Energy through the Energy Storage Program in the Office of Electricity. We acknowledge Dr. Jagjit Nanda SLAC National Accelerator Laboratory for the fruitful discussions.

Novel indium phosphide charged particle detector characterization with a 120 GeV proton beam

Thin film detectors which incorporate semiconductor materials other than silicon have the potential to build upon their unique material properties and offer advantages such as faster response times, operation at room temperature, and radiation hardness. To explore the possibility, promising candidate materials were selected, and particle tracking detectors were fabricated. An indium phosphide detector with a metal-intrinsic-metal structure has been fabricated for particle tracking. The detector was tested using radioactive sources and a high energy proton beam at Fermi National Accelerator Laboratory. In addition to its simplistic design and fabrication process, the indium phosphide particle detector showed a very fast response time of hundreds of picoseconds for the 120 GeV protons, which are comparable to the ultra-fast silicon detectors. This fast-timing response is attributed to the high electron mobility of indium phosphide. Such material properties can be leveraged to build novel detectors with superlative performance.

Development of an X-ray ionization beam position monitor for PAL-XFEL soft X-rays.

The Pohang Accelerator Laboratory X-ray Free-Electron Laser (PAL-XFEL) operates hard X-ray and soft X-ray beamlines for conducting scientific experiments providing intense ultrashort X-ray pulses based on the self-amplified spontaneous emission (SASE) process. The X-ray free-electron laser is characterized by strong pulse-to-pulse fluctuations resulting from the SASE process. Therefore, online photon diagnostics are very important for rigorous measurements. The concept of photo-absorption and emission using solid materials is seldom considered in soft X-ray beamline diagnostics. Instead, gas monitoring detectors, which utilize the photo-ionization of noble gas, are employed for monitoring the beam intensity. To track the beam position at the soft X-ray beamline in addition to those intensity monitors, an X-ray ionization beam position monitor (XIBPM) has been developed and characterized at the soft X-ray beamline of PAL-XFEL. The XIBPM utilizes ionization of either the residual gas in an ultra-high-vacuum environment or injected krypton gas, along with a microchannel plate with phosphor. The XIBPM was tested separately for monitoring horizontal and vertical beam positions, confirming the feasibility of tracking relative changes in beam position both on average and down to single-shot measurements. This paper presents the basic structure and test results of the newly developed non-invasive XIBPM.

An MeV Proton Irradiation Facility: DICE.

Materials applied in nuclear environments such as fission or fusion power-plants face severe conditions. The irradiation by neutrons induces thermal loads and irradiation damage. Furthermore, coolants in contact with the materials induce corrosion, which is particularly challenging for liquid salts intended for the next generation of fission reactors. A new device (DICE) is installed at the 3.5 MV accelerator at DIFFER for the accelerated testing of such materials under combined irradiation and corrosion conditions. The DICE enables irradiation of samples at temperatures of up to 1050 K and in contact with liquid salts. An integrated shielding and a low power temperature control concept based on radiation cooling enables high-duty cycle application in a standard accelerator laboratory. Ion currents of up to 30 µA are possible with continuous irradiation. This work outlines the technical concept of the device and presents the first data.

Optimizing High-Throughput Inference on Graph Neural Networks at Shared Computing Facilities with the NVIDIA Triton Inference Server

With machine learning applications now spanning a variety of computational tasks, multi-user shared computing facilities are devoting a rapidly increasing proportion of their resources to such algorithms. Graph neural networks (GNNs), for example, have provided astounding improvements in extracting complex signatures from data and are now widely used in a variety of applications, such as particle jet classification in high energy physics (HEP). However, GNNs also come with an enormous computational penalty that requires the use of GPUs to maintain reasonable throughput. At shared computing facilities, such as those used by physicists at Fermi National Accelerator Laboratory (Fermilab), methodical resource allocation and high throughput at the many-user scale are key to ensuring that resources are being used as efficiently as possible. These facilities, however, primarily provide CPU-only nodes, which proves detrimental to time-to-insight and computational throughput for workflows that include machine learning inference. In this work, we describe how a shared computing facility can use the NVIDIA Triton Inference Server to optimize its resource allocation and computing structure, recovering high throughput while scaling out to multiple users by massively parallelizing their machine learning inference. To demonstrate the effectiveness of this system in a realistic multi-user environment, we use the Fermilab Elastic Analysis Facility augmented with the Triton Inference Server to provide scalable and high-throughput access to a HEP-specific GNN and report on the outcome.

Practices and Rules of 16th Century Genoese Gilding: Exploring Gold Leaf Thickness and Caratage through X-ray and Ion Beam Techniques

This study investigates the practices and rules of Genoese gilding, drawing insights from a 16th-century manuscript containing regulations for gold leaf production. Employing X-ray and ion beam techniques, we quantitatively assess the manuscript’s gold leaf thickness without destructive sampling. Artisanal goldbeater-produced leaves of different thicknesses, applied with a guazzo or mordant technique, served as standards. Further analysis of samples with unknown thickness from the furniture of Palazzo Spinola di Pellicceria in Genoa (Italy) has confirmed the method’s applicability to practical cases. External beam Rutherford backscattering spectrometry (RBS) and particle-induced X-ray emission (PIXE) analyses were carried out using 3 MeV protons at the LABEC accelerator laboratory in Florence. A linear relationship between Gold Lα peak yield and leaf thickness, as measured by RBS, has been established for optimal calibration of portable or hand-held X-Ray fluorescence (XRF) instrumentation for in situ measurements. Moreover, the caratage of the gold foil preserved in the manuscript has been assessed.

X-ray optics for the cavity-based X-ray free-electron laser.

A cavity-based X-ray free-electron laser (CBXFEL) is a possible future direction in the development of fully coherent X-ray sources. CBXFELs consist of a low-emittance electron source, a magnet system with several undulators and chicanes, and an X-ray cavity. The X-ray cavity stores and circulates X-ray pulses for repeated FEL interactions with electron pulses until the FEL reaches saturation. CBXFEL cavities require low-loss wavefront-preserving optical components: near-100%-reflectivity X-ray diamond Bragg-reflecting crystals, outcoupling devices such as thin diamond membranes or X-ray gratings, and aberration-free focusing elements. In the framework of the collaborative CBXFEL research and development project of Argonne National Laboratory, SLAC National Accelerator Laboratory and SPring-8, we report here the design, manufacturing and characterization of X-ray optical components for the CBXFEL cavity, which include high-reflectivity diamond crystal mirrors, a diamond drumhead crystal with thin membranes, beryllium refractive lenses and channel-cut Si monochromators. All the designed optical components have been fully characterized at the Advanced Photon Source to demonstrate their suitability for the CBXFEL cavity application.

The photodissociation dynamics and ultrafast electron diffraction image of cyclobutanone from the surface hopping dynamics simulation

The comprehension of nonadiabatic dynamics in polyatomic systems relies heavily on the simultaneous advancements in theoretical and experimental domains. The gas-phase ultrafast electron diffraction (UED) technique has attracted significant attention as a unique tool for monitoring photochemical and photophysical processes at the all-atomic level with high temporal and spatial resolutions. In this work, we simulate the UED spectra of cyclobutanone using the trajectory surface hopping method at the extended multi-state complete active space second order perturbation theory (XMS-CASPT2) level and thereby predict the results of the upcoming UED experiments in the Stanford Linear Accelerator Laboratory. The simulated results demonstrate that a few pathways, including the C2 and C3 dissociation channels, as well as the ring opening channel, play important roles in the nonadiabatic reactions of cyclobutanone. We demonstrate that the simulated UED signal can be directly interpreted in terms of atomic motions, which provides a unique way of monitoring the evolution of the molecular structure in real time. Our work not only provides numerical data that help to determine the accuracy of the well-known surface hopping dynamics at the high XMS-CASPT2 electronic-structure level but also facilitates the understanding of the microscopic mechanisms of the photoinduced reactions in cyclobutanone.