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At least 667 records · Page 37

Enhancing the mass resolving power of FRIB’s proposed high-voltage MR-ToF mass separator and spectrometer: Addressing non-ideal conditions

Multi-reflection time-of-flight mass separators and spectrometers (MR-ToF MSs) are indispensable tools at radioactive ion beam (RIB) facilities. These electrostatic ion beam traps act as highly selective mass separators and high-precision mass spectrometers for rare and exotic nuclei. When well-tuned and designed to minimize higher-order flight-time aberrations, state-of-the-art MR-ToF MSs approach, and slightly exceed, mass resolving powers of m/Δm = 10 6 . Achieving m/Δm ≥ 3 ⋅ 10 6 would provide the ability to resolve > 90 % of all known isomeric states with half-lives above 10 ms. However, the ability to mass separate in all practical setups is limited by non-ideal conditions which place such resolving powers out of reach. Here, to this end, we present a simulated analysis of these conditions in the newly proposed high-voltage MR-ToF MS for the Facility for Rare Isotope Beams (FRIB). It is expected to store ions at 30 keV beam energy and increase ion throughput by two orders of magnitude compared to current devices. Existing efforts to mitigate the effects of non-ideal conditions employed for current MR-ToF devices storing ions at < 3 keV beam energy will already enable mass resolving powers approaching 10 6 for FRIB’s high-voltage MR-ToF device. Simulations of newly proposed mitigation strategies show that even mass resolving powers approaching 10 7 might become feasible.

Electrostatic ion beam traps↗

The BigBite Calorimeter for the Super Bigbite Spectrometer Program at Jefferson Lab

Here, we report features of the design, construction, installation, and performance of the BigBite Calorimeter (BBCal), a lead-glass electromagnetic calorimeter constructed as part of the BigBite Spectrometer (BBS), which served as the electron arm for the Super Bigbite Spectrometer (SBS) program of high-precision neutron electromagnetic form factor measurements in Hall A at Jefferson Lab. As a total-absorption calorimeter, BBCal provided the primary electron trigger for BBS, detecting quasi-elastically scattered electrons in the 1–4 GeV energy range with an energy resolution of approximately 6.2%, position resolution of 1.2 cm, and timing resolution of 0.5 ns.

BBCal↗

Performance of the Particle-Identification Silicon-Telescope Array coupled with the VAMOS++ magnetic spectrometer

The Particle-Identification Silicon-Telescope Array (PISTA) is a new detection system designed for high-resolution studies of fission process induced by multi-nucleon transfer in inverse kinematics. It is specifically optimized for experiments with the VAMOS++ magnetic spectrometer at GANIL (Grand Accélérateur National d’Ions Lourds). The array comprises eight trapezoidal ΔE-E silicon telescopes arranged in a lamp shade configuration. Each telescope integrates two single-sided stripped silicon detectors, enabling target-like recoil identification, energy loss measurements, and trajectory reconstruction. Positioned in close proximity to the target, PISTA’s compact geometry achieves high-efficiency tracking of target-like recoils produced in multi-nucleon transfer reactions at Coulomb barrier energies. The spatial segmentation of the array allows precise determination of the mass and charge of the target-like nucleus, and excitation energy of fissioning systems. This work presents the particle identification and excitation energy reconstruction performances for the interactions of 238 U beam with 12 C target. An excitation energy resolution of 800 keV (FWHM) was determined together with mass resolution of 1.1% (FWHM). The combination of PISTA and VAMOS++ magnetic spectrometer enables unprecedented investigations of the fission process as a function of the excitation energy of the fissioning nucleus, particularly for exotic systems produced in transfer-induced reactions.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Initial Characterization and Optimization of the Liquid Sampling-Atmospheric Pressure Glow Discharge Ionization Source Coupled to an Orbitrap Mass Spectrometer for the Determination of Plutonium

Plutonium measurements are essential to the nuclear forensics and safeguards community. The liquid sampling-atmospheric pressure glow discharge (LS-APGD) microplasma ionization source coupled with an Orbitrap mass spectrometer is a proven platform for uranium isotope ratio determinations. Here, this work expands the LS-APGD-Orbitrap platform capabilities by reporting the first-ever analysis of plutonium with the LS-APGD and the first-ever measurement of elemental plutonium with an Orbitrap mass spectrometer. This coupling has the potential to dramatically reduce the complex sample manipulations required for traditional analysis techniques employed for actinide isotope ratio determinations. As a first step toward the goal of simultaneous uranium and plutonium isotope ratio determinations, the initial characterization and optimization of the platform for the detection of plutonium are reported. Collision-induced dissociation modality settings were optimized to reduce water-related and other molecular clusters containing plutonium, maximizing 242 Pu 16 O 2 + responses. A design of experiments study was conducted to optimize the discharge conditions of the dual-electrode LS-APGD toward the responsivity of 242 Pu 16 O 2 +. The measurement sensitivity was determined from a Pu response curve, yielding a limit of detection of 10 fg (absolute) of total analyte when data was collected and processed with a Spectroswiss FTMS Booster X2 data acquisition system. Additionally, plutonium and uranium were measured in a simultaneous acquisition, and each analyte remained unaffected by the other. It is believed that the LS-APGD-Orbitrap platform could be a valuable addition to the nuclear forensics’ toolbox and, indeed, other scientific disciplines and regulatory communities in which rapid, high-resolution plutonium determinations are paramount.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Sensitive Mass Spectrometer for Time-Resolved Gas-Phase Chemistry Studies at High Pressures

Here, we report the construction of a new experimental apparatus for direct time-resolved probing of high-pressure gas-phase chemical reactions by photoionization mass spectrometry. The apparatus uses a laser photolysis slow-flow reactor, capable of operating at P = 0.3 — 100 bar and T = 300 — 1000 K. In this report, we initiate reactions in homogeneous gas mixtures by the photolysis of appropriate radical precursor using laser pulses at repetition rates of 1 — 10 Hz. The reacting mixture is continuously sampled into a vacuum chamber, ionized by VUV photons from laboratory-based discharge lamps or from a synchrotron beamline, and analyzed by a custom-designed mass spectrometer. Soft near-threshold ionization by tunable synchrotron radiation enables spectroscopic quantification of many key intermediates and products of chemical reactions. A novel ionization scheme in the high-density region of the sample gas jet increases the experimental sensitivity 100-fold, compared with existing instruments, without compromising mass resolution. A 40-kHz pulsed reflectron time-of-flight mass spectrometer in the orthogonal acceleration geometry achieves simultaneous detection of all ionized species with 25-μs time resolution. We show the power of this apparatus by investigating the ethyl radical oxidation reaction using very dilute (<10 12 molecules • cm -3 ) ethyl concentrations at pressures up to 25 bar.

47 OTHER INSTRUMENTATION↗

High Mass Analysis with a Fourier Transform Ion Cyclotron Resonance Mass Spectrometer: From Inorganic Salt Clusters to Antibody Conjugates and Beyond

Analysis of proteins and complexes under native mass spectrometric (MS) and solution conditions was typically performed using time-of-flight (ToF) analyzers, due to their routine high m/z transmission and detection capabilities. However, over recent years, the ability of Orbitrap-based mass spectrometers to transmit and detect a range of high molecular weight species is well documented. Herein, we describe how a 15 Tesla Fourier transform ion cyclotron resonance mass spectrometer (15 T FT-ICR MS) is more than capable of analyzing a wide range of ions in the high m/z scale (>5000), in both positive and negative instrument polarities, ranging from the inorganic cesium iodide salt clusters; a humanized IgG1k monoclonal antibody (mAb; 148.2 kDa); an IgG1-mertansine drug conjugate (148.5 kDa, drug-to-antibody ratio; DAR 2.26); an IgG1-siRNA conjugate (159.1 kDa; ribonucleic acid to antibody ratio; RAR 1); the membrane protein aquaporin-Z (97.2 kDa) liberated from a C8E4 detergent micelle; the empty MSP1D1-nanodisc (142.5 kDa) and the tetradecameric chaperone protein complex GroEL (806.2 kDa; GroEL dimer at 1.6 MDa). We also investigate different regions of the FT-ICR MS that impact ion transmission and desolvation. Finally, we demonstrate how the transmission of these species and resultant spectra are highly consistent with those previously generated on both quadrupole-ToF (Q-ToF) and Orbitrap instrumentation. This article serves as an impactful example of how FT-ICR mass analyzers are competitive to Q-ToFs and Orbitraps for high mass detection at high m/z.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

A Flat Analyzer Polycapillary Spectrometer for X-ray Absorption Spectroscopy of Dilute Transition Metals at X-ray-Free Electron Lasers

X-ray absorption spectroscopy (XAS) coupled with highly intense pulses from an X-ray-free electron laser (XFEL) can be used to track ultrafast chemical dynamics. Nonetheless, measurements for dilute samples (≤1 mM) have been exceptionally challenging, as scattering background signals dominate over the sample’s X-ray fluorescence. We show that femtosecond time-resolved XAS measurements of sub-millimolar transition metal solutions are now possible at the Linac Coherent Light Source (LCLS) using a high-throughput polycapillary XAS spectrometer, designed, developed, and commissioned at LCLS and the Stanford Synchrotron Radiation Lightsource (SSRL). The instrument integrates three polycapillary optics that collect and collimate X-ray fluorescence emitted from the interaction point with a high solid angle. X-ray collimated fluorescence is then selectively diffracted by coupled graphite analyzer crystals. As a result, the contribution of scattered photons is suppressed. Experiments at the Pt L 3 -edge on 0.1 mM aqueous K 2 PtCl 6 (delivered via a 100 μm liquid jet) were successfully performed in the laser pump X-ray probe configuration at the LCLS XCS and XPP instruments. We report the transient spectra of hexachloroplatinate within the first 10 ps after a 266 nm photoexcitation. We observed a short-lived reduced intermediate (≈2 ps). The polycapillary X-ray spectrometer at LCLS now enables the efficient study of the dynamics of ultradilute transition metals in solution. This capability opens the door to investigating plasmonic systems, photocatalysts, enzymes, and other scarce and dilute samples.

LCLS↗

Compact folded metasurface spectrometer

Abstract An optical design space that can highly benefit from the recent developments in metasurfaces is the folded optics architecture where light is confined between reflective surfaces, and the wavefront is controlled at the reflective interfaces. In this manuscript, we introduce the concept of folded metasurface optics by demonstrating a compact spectrometer made from a 1-mm-thick glass slab with a volume of 7 cubic millimeters. The spectrometer has a resolution of ~1.2 nm, resolving more than 80 spectral points from 760 to 860 nm. The device is composed of three reflective dielectric metasurfaces, all fabricated in a single lithographic step on one side of a substrate, which simultaneously acts as the propagation space for light. The folded metasystem design can be applied to many optical systems, such as optical signal processors, interferometers, hyperspectral imagers, and computational optical systems, significantly reducing their sizes and increasing their mechanical robustness and potential for integration.

47 OTHER INSTRUMENTATION↗

Sample changers for direct geometry neutron chopper spectrometers

The advent of higher flux neutron sources has made the use of sample changers appropriate across the instrument suites at neutron scattering facilities. We examine the efficiency, design, and operation of two sample changers used at the thermal chopper spectrometers at the Spallation Neutron Source. We also present case studies of sample holders designed to accommodate multiple single crystal or powder samples for the Cold Neutron Chopper Spectrometer at the Spallation Neutron Source. [This manuscript has been authored by UT-Battelle, LLC under Contract No. DE-AC05-00OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (http://energy.gov/downloads/doe-public-access-plan).]

Stone, Matthew B. [Oak Ridge National Laboratory (↗

Tritium targets for use in solenoidal spectrometers

Nucleon adding and removing reactions are an ideal probe to study the single-particle foundations of nuclear structure. For experiments far away from the valley of stability, one needs to use radioactive beams in inverse kinematics. To maintain excellent resolution, solenoidal spectrometers like HELIOS at Argonne National Laboratory (ANL), ISS at CERN or SOLARIS at the Facility for Rare Isotope Beams (FRIB) are used. Typically, deuterated plastic foils are the targets of choice. Depending on the energy deposited, these targets might degrade quickly in beam. The potential of using tritium-implanted targets in conjunction with the solenoidal spectrometers was realized for access to even more exotic nuclei with outstanding resolving power. While no tritiated polyethylene is commercially available at the moment, tritium-containing titanium targets have been produced in the past. Unfortunately the loading fraction of tritium for the latter was often very low and not reproducible. The progress in the production of tritium-containing targets is presented, including the characterization of the foils.

Müller-Gatermann, Claus↗

Investigations of 2β decay measured by low background HPGe spectrometer OBELIX

A low background high sensitive HPGe spectrometer OBELIX was installed at the Modane Underground Laboratory (LSM, France, 4800 m w.e.). The detector was designed to measure a contamination of enriched isotopes and radio-impurities in construction materials, to investigate rare nuclear processes such as resonance neutrinoless double electron capture and two-neutrino double beta decay to excited states of daughter nuclei. Spectrometer sensitivity, contamination of NEMO-3 sources and results of 2ν2β{sup −} decay of {sup 100}Mo to the 0{sup +} (1130 keV) and 2{sup +} (540 keV) excited states as well as future plans for OBELIX detector are given.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

A stretch/compress scheme for a high temporal resolution detector for the magnetic recoil spectrometer time (MRSt)

Here we present a time-resolved detector concept for the magnetic recoil spectrometer for time-resolved measurements of the NIF neutron spectrum. The measurement is challenging due to the time spreading of the recoil protons (or deuterons) as they transit an energy dispersing magnet system. Ions arrive at the focal plane of the magnetic spectrometer over an interval of tens of nanoseconds. We seek to measure the time-resolved neutron spectrum with 20 ps precision by manipulating an electron signal derived from the ions. A stretch-compress scheme is employed to remove transit time skewing while simultaneously reducing the bandwidth requirements for signal recording. Simulation results are presented along with design concepts for structures capable of establishing the required electromagnetic fields.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Calibration of the microcalorimeter spectrometer on-board the Hitomi (Astro-H) observatory (invited)

The Hitomi Soft X-ray Spectrometer (SXS) was a pioneering non-dispersive imaging x-ray spectrometer with 5 eV FWHM energy resolution, consisting of an array of 36 silicon-thermistor microcalorimeters at the focus of a high-throughput soft x-ray telescope. Here, the instrument enabled astrophysical plasma diagnostics in the 0.3–12 keV band. We introduce the SXS calibration strategy and corresponding ground calibration measurements that took place from 2012–2015, including both the characterization of the microcalorimeter array and measurements of the x-ray transmission of optical blocking filters.

47 OTHER INSTRUMENTATION↗

Calibration and characterization of a highly efficient spectrometer in von Hamos geometry for 7-10 keV x-rays

Here, we have built an absolutely calibrated, highly efficient, Bragg crystal spectrometer in von Hamos geometry. This zinc von Hamos spectrometer uses a crystal made from highly oriented pyrolytic graphite that is cylindrically bent along the non-dispersive axis. It is tuned to measure x-ray spectra in the 7–10 keV range and has been designed to be used on a Ten Inch Manipulator for the Omega and OmegaEP target chambers at the Laboratory for Laser Energetics in Rochester, USA. Significant shielding strategies and fluorescence mitigation have been implemented in addition to an imaging plate detector making it well suited for experiments in high-intensity environments. Here we present the design and absolute calibration as well as mosaicity and integrated reflectivity measurements.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Near shot-noise limited time-resolved circular dichroism pump-probe spectrometer

We describe an optical near shot-noise limited time-resolved circular dichroism (TRCD) pump-probe spectrometer capable of reliably measuring circular dichroism signals in the order of $\mu$deg with nanosecond time resolution. Such sensitivity is achieved through a modification of existing TRCD designs and introduction of a new data processing protocol that eliminates approximations that have caused substantial nonlinearities in past measurements and allows the measurement of absorption and circular dichroism transients simultaneously with a single pump pulse. The exceptional signal-to-noise ratio of the described setup makes the TRCD technique applicable to a large range of non-biological and biological systems. Finally, the spectrometer was used to record, for the first time, weak TRCD kinetics associated with the triplet state energy transfer in the photosynthetic Fenna-Matthews-Olson antenna pigment-protein complex.

47 OTHER INSTRUMENTATION↗

Measurement of apparent ion temperature using the magnetic recoil spectrometer at the OMEGA laser facility

The Magnetic Recoil neutron Spectrometer (MRS) at the OMEGA laser facility has been routinely used to measure deuterium-tritium (DT) yield and areal density in cryogenically layered implosions since 2008. Recently, operation of the OMEGA MRS in higher-resolution mode with a new smaller, thinner (4 cm 2 , 57 μm thick) CD 2 conversion foil has also enabled inference of the apparent DT ion temperature (T ion ) from MRS data. MRS-inferred T ion compares well with T ion as measured using neutron time-of-flight spectrometers, which is important as it demonstrates good understanding of the very different systematics associated with the two independent measurements. The MRS resolution in this configuration, $ΔE_{MRS}$ = 0.91 MeV FWHM, is still higher than that required for a high-precision T ion measurement. We show herein how fielding a smaller foil closer to the target chamber center and redesigning the MRS detector array could bring the resolution to $ΔE_{MRS}$ = 0.45 MeV, reducing the systematic T ion uncertainty by more than a factor of 4.

47 OTHER INSTRUMENTATION↗

Instrumentation for the upgrade to the JET core charge-exchange spectrometers

Charge-exchange spectroscopy on JET has become particularly challenging with the introduction of the ITER-like wall. The line intensities are weaker and contaminated by many nuisance lines. We have therefore upgraded the instrumentation to improve throughput and allow the simultaneous measurement of impurity and fuel-ion charge exchange by splitting the light between two pairs of imaging spectrometers using dichroic beam splitters. Imaging instruments allow us to stack 11 × 1 mm diameter fibres on the entrance slits without cross talk. CCD cameras were chosen to have 512 × 512 pixels to allow frame transfer times <0.2 ms which with minimum exposure times of 5 ms give tolerable smearing even without a chopper. The image plane is optically demagnified 2:1 to match the sensor size of these cameras. Because the image plane of the spectrometer is tilted, the CCD must also be tilted to maintain focus over the spectrum (Scheimpflug condition). To avoid transverse keystoning (causing the vertical height of the spectra to change across the sensor), the configuration is furthermore designed to be telecentric by a suitable choice of the lens separation. The lens configuration is built almost entirely from commercial off-the-shelf components, which allowed it to be assembled and aligned relatively rapidly to meet the deadline for in-vessel calibration in the JET shutdown.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

The Warm Electron Beam Ion Trap (WEBIT): An instrument for ground calibration of space-borne x-ray spectrometers

The warm electron beam ion trap (WEBIT) at Lawrence Livermore National Laboratory is being developed as a pre-launch, ground calibration source for space-borne, high-throughput, high-resolution x-ray spectrometers, such as the x-ray imaging and spectroscopy mission Resolve quantum calorimeter. Historically, calibration sources for calorimeter spectrometers have relied on characteristic line emission from x-ray tubes, fluorescing metals, and radioactive sources. The WEBIT, by contrast, relies on emission from x-ray transitions in highly charged ions, for example, hydrogen-like and helium-like ions, whose energies are well known and whose line shapes are relatively simple. The WEBIT can create astrophysically relevant ions whose x-ray emission falls in the 0.3-12 keV science bandpass of Resolve and has a portable design advantageous for a calibration source. The WEBIT will be used to help calibrate Resolve’s instrumental line shape and gain scale as a function of various operational parameters during both detector subsystem level testing and instrumental level testing.

47 OTHER INSTRUMENTATION↗