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DOE OSTI2026

Resonance Ionization Spectroscopy Experiment at Facility for Rare Isotope Beams

This manuscript reports on the commissioning of the Resonance Ionization Spectroscopy Experiment (RISE) at the BEam COoler and LAser spectroscopy (BECOLA) facility at Facility for Rare Isotope Beams (FRIB). The instrument implements the collinear resonance ionization spectroscopy technique for sensitive measurements of isotope shifts and hyperfine structure of short-lived isotopes produced at FRIB. The existing BECOLA beamline was extended to integrate an electrostatic ion-beam bender and an ion detector at ultrahigh vacuum. An injection-seeded titanium-sapphire laser and a multiharmonic pulsed neodymium-doped yttrium aluminum garnet laser were installed to perform resonant excitation and selective ionization. Commissioning tests were performed to demonstrate the capabilities of the instrument by measuring the hyperfine structure of stable 27 Al produced in an offline ion source. The RISE instrument is ready and operational for future studies of short-lived isotopes at FRIB.

Atomic spectra↗

DOE OSTI2025

Versatile system for ion energy measurements generated by pulsed laser ionization: Insights into electron-ion dynamics

Ion energy distributions generated by pulsed laser interactions with materials are essential for applications ranging from materials science to oncology. Ion energy characterization is particularly important for an emerging mass spectrometry technique called virtual-slit cycloidal mass spectrometry (VS-CMS). The ion energy distribution influences the design and performance of VS-CMS instruments, as well as the efficacy of laser-driven ionization methods in various fields. Several established techniques, including the retarding potential method, time-of-flight (TOF) analysis, and electrostatic energy analyzers, have been employed to measure ion energy distributions. The wide range of ion energies reported highlights the strong dependence of ion energy on laser parameters, target materials, and experimental conditions, as well as the necessity of making independent measurements of the ion energy distribution for specific laser systems and materials. This paper presents the design and characterization of a simple TOF-based apparatus for measuring ion energy distributions from pulsed laser ionization without external fields. This approach minimizes perturbation of electron-ion dynamics and enables simultaneous energy measurements at multiple spatial positions. Here, the apparatus was tested using a nanosecond pulsed Nd:YAG laser operating at 1064 nm, 532 nm, and 266 nm on solid copper sheets at various laser fluences. Simultaneous measurements at different distances provide new insights into ion-electron interactions post-ionization and demonstrate the influence of laser wavelength and fluence on ion energy distributions.

Ion energy↗

DOE OSTI2025

Shear Response of Ionizable Polymer Melts at the Crossover from Ionomers to Polyelectrolytes

Nonlinear shear response of polymers is affected by inherent barriers for diffusive motion, including entanglements and topology. In ionizable polymers, ionic clusters further constrain the intrinsic dynamics of the polymers, significantly enhancing their viscosity. Here, using fully atomistic molecular dynamics simulations, the nonlinear shear response of ionizable polymers is presented, across the transition from the ionomer regime where distinctive clusters dominate the structure to the polyelectrolyte regime where clusters percolate, in polystyrene randomly sulfonated with fractions of SO 3 − groups of f = 0.20 and 0.35, in pristine and tetrahydrofuran (THF) swollen polyelectrolyte melts. For f = 0.20, the ionic clusters first fracture into smaller clusters followed by splitting into individual ionic groups and eventually reform. At higher f, the clusters morph in shape but do not break under high shear. At very high shear rates, all of the chains stretch and recoil rapidly. As the shear rate is reduced, some chains stretch and recoil, while others remain largely unaffected by the shear. Macroscopically, for all systems, the shear viscosity displays initially an elastic response, followed by nonlinear shear stress overshoot and, eventually, a steady state. The evolution of viscosity with time and shear reflects that of the ionizable domains.

cluster chemistry↗

DOE OSTI2025

Impact of ionization peak location on measured opaqueness in DIII-D H-mode plasmas

This study investigates the relationship between electron pedestal density and the location of the ionization peak on neutral penetration in DIII-D H-mode plasmas, utilizing a database of Lyman-α emission measurements. The high electron density leads to neutrals being ‘screened’ and the ionization front being pushed out into the Scrape-Off Layer (SOL). This is also referred to as the neutral opaqueness, which is heuristically expected to scale with edge plasma density and machine size. However, at lower electron pedestal density, the penetration depth of the neutrals varies, and measured opaqueness deviates from the heuristic scaling. The database reveals that at low density, when the ionization peak is located in SOL region, the linear relationship between the electron density and neutral penetration holds. However, when the peak is located inside the separatrix, the penetration of the neutrals (λ n 0 ) is much wider ~3.0–3.5 cm, breaking the heuristic opaqueness approximation. These findings provide valuable insights into fueling efficiency and plasma behavior, with implications for Fusion Pilot Plants where high pedestal densities are anticipated and where the neutral opaqueness behaves like its heuristic approximation. This analysis offers a framework to refine neutral opaqueness approximations, enhancing the predictive capability for advanced tokamak operations.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2026

Ionization and temperature measurements in warm dense copper using x-ray absorption spectroscopy

We detail experimental results inferring ionization and temperature for warm dense copper plasmas at several times solid density (15–25 g/cm 3 ) and temperatures of 10–21 eV. Experiments performed at the OMEGA Laser Facility generate uniform warm dense matter conditions via symmetric shock compression of a buried copper layer. The plasma is probed with a laser-generated x-ray source to collect the K-shell x-ray absorption spectrum. Fitting bound-bound absorption contributions from constituent charge states of copper provides an estimated $\overline{Z}$ of approximately 4–7 for these warm dense copper plasmas. We find that these partially ionized plasmas have K-edge shifts of 12–30 eV and bound-bound resonance 1s → 3p absorption shifts of 4–26 eV with respect to the cold K edge. This study provides necessary experimental data to improve ionization and opacity models in the warm dense matter regime.

42 ENGINEERING↗

DOE OSTI2025

Particle composition measurements for ultrafine particles collected at the EPCAPE Mount Soledad site from 04-27-2023 to 06-13-2023 using a Thermal Desorption Chemical Ionization Mass Spectrometer

The dataset contains particle composition data for both the positive and negative reagent ion modes of the Thermal Desorption Chemical Ionization Mass Spectrometer (TDCIMS). The dataset is split into two directories: one for particles with diameters of 30 nm and the other for particles with diameters of less than 100 nm. The positive reagent ion mode uses H3O+ as the reagent ion, and ionization usually occurs through hydrogen addition. The negative mode uses O2- as the reagent ion. Negative mode ionization generally occurs through hydrogen abstraction, but O2- addition is also possible. Ion concentrations were normalized to total ion counts, and unknown ions were then removed from the data. The name of each ion fraction time series includes the mass to charge ratio and the chemical formula for the ion. Time is recorded in seconds since 1/1/1904. The time zone is UTC.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2026

Exploring Approaches for Accelerated Mass Spectrometric Detection of Fluorochemicals from Aqueous Solutions Using Indirect, Adsorbent-Facilitated Desorption Ionization

There is a growing need for rapid, low-cost analytical tools to screen water supplies for persistent contaminants. Due to their ubiquitous presence in the environment and their detrimental effects on human health, there is a public interest in widespread testing for perfluoroalkyl substances (PFAS). However, the most common methods for PFAS analysis can be time-intensive, requiring a preconcentration step followed by liquid chromatography–mass spectrometry (LC–MS), and are cost-prohibitive for most members of the public. To address these challenges, this study explores a novel method for rapid analysis of aqueous analytes by concentrating analytes on solid adsorbents and detecting them using mass spectrometric analysis via desorption ionization directly from the adsorbent surface. We demonstrate this general approach of indirect solution analysis (ISA) with desorption electrospray ionization (ISA-DESI) and laser desorption ionization (ISA-LDI). Various adsorbent materials were screened, including commercial mesoporous carbons, alumina, and metal–organic frameworks (MOFs). Using ISA-DESI, we consistently detect concentrations as low as 5–100 parts per trillion (ppt) for perfluorooctanoic acid (PFOA) and 10–100 ppt for perfluoroundecanoic acid (PFUnDA). This approach enables rapid detection in under 5 min, making it suitable for applications requiring trace detection with fast response times. We further demonstrate the use of ISA-DESI on a range of environmentally relevant contaminants. Advantages of this indirect solution analysis approach include simplified sample preparation, accelerated analysis, and low cost with readily available materials, making it a promising tool to accelerate mass spectrometric PFAS detection for identifying contaminated sites, performing laboratory studies, and monitoring industrial waste streams.

Bays, Nathan Robert [Sandia National Laboratories ↗

DOE OSTI2024

Actinide Elemental Ratios of Spent Nuclear Fuel Samples by Resonance Ionization Mass Spectrometry

While resonance ionization mass spectrometry (RIMS) has demonstrated utility in measuring isotopic compositions of elements in complex matrices without the need for chemical separation to remove isobaric interferences, it has had limited application in measuring elemental compositions. The ability to determine elemental compositions via an in situ method like RIMS would be an exceptional asset in spent nuclear fuel analysis, where they are important in assessing reactor histories and whose chemical separation presents a radiological hazard. However, quantitative elemental analysis by RIMS requires special considerations because each element is ionized by its own set of lasers tuned to element specific resonant ionization wavelengths. We present the first comprehensive study of measuring elemental ratios by RIMS in spent nuclear fuel. All actinides produced by neutron capture are enhanced significantly radially from the center to the edge of a fuel pellet. This edge effect is not readily accessible by conventional bulk measurements.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2024

Transverse emittance reduction in muon beams by ionization cooling

Accelerated muon beams have been considered for the next-generation studies of high-energy lepton–antilepton collisions and neutrino oscillations. However, high-brightness muon beams have not yet been produced. The main challenge for muon acceleration and storage stems from the large phase-space volume occupied by the beam, derived from the production mechanism of muons through the decay of pions. The phase-space volume of the muon beam can be decreased through ionization cooling. Here we show that ionization cooling leads to a reduction in the transverse emittance of muon beams that traverse lithium hydride or liquid hydrogen absorbers in the Muon Ionization Cooling Experiment. Our results represent a substantial advance towards the realization of muon-based facilities that could operate at the energy and intensity frontiers.

43 PARTICLE ACCELERATORS↗

DOE OSTI2024

Collective excitations and low-energy ionization signatures of relativistic particles in silicon detectors

Abstract Solid-state detectors with a low energy threshold have several applications, including searches of non-relativistic halo dark-matter particles with sub-GeV masses. When searching for relativistic, beyond-the-Standard-Model particles with enhanced cross sections for small energy transfers, a small detector with a low energy threshold may have better sensitivity than a larger detector with a higher energy threshold. In this paper, we calculate the low-energy ionization spectrum from high-velocity particles scattering in a dielectric material. We consider the full material response including the excitation of bulk plasmons. We generalize the energy-loss function to relativistic kinematics, and benchmark existing tools used for halo dark-matter scattering against electron energy-loss spectroscopy data. Compared to calculations commonly used in the literature, such as the Photo-Absorption-Ionization model or the free-electron model, including collective effects shifts the recoil ionization spectrum towards higher energies, typically peaking around 4–6 electron-hole pairs. We apply our results to the three benchmark examples: millicharged particles produced in a beam, neutrinos with a magnetic dipole moment produced in a reactor, and upscattered dark-matter particles. Our results show that the proper inclusion of collective effects typically enhances a detector’s sensitivity to these particles, since detector backgrounds, such as dark counts, peak at lower energies.

Physics↗

DOE OSTI2025

Time-resolved momentum imaging of UV photodynamics in structural isomers of iodopropane probed by site-selective XUV ionization

The photodynamics of 1- and 2-iodopropane (1 and 2-IP) were studied in a time-resolved scheme incorporating ultraviolet (UV) excitation and extreme ultraviolet (XUV) probing, which initiates photoionization selectively from the I 4d core orbital. UV absorption in the A-band of both isomers leads to prompt C–I bond fission, with significant disposal of internal energy into the propyl radical product. Site-selective ionization enables a range of charge transfer (CT) processes between the nascent highly charged iodine ions and neutral propyl radicals, dependent on the interfragment distance at the instant of ionization. Subtle differences in the dynamics of these CT processes between the two isomers are observed. In 1-IP, the kinetic energies of iodine ions produced by UV photodissociation and subsequent XUV multiple ionization increased notably over the first few hundred femtoseconds, which could be understood in terms of differing gradients along the photodissociation coordinates of the neutral and polycationic states involved in the pump and probe steps, respectively. Led by a recent report of HI elimination in UV photoexcited 2-IP [Todt et al., Phys. Chem. Chem. Phys., 22(46), 27338 (2020)], we also model the most likely signatures of this process in the present experiment, and can identify signal in the 2-IP data (that is absent or significantly weaker in the data from the unbranched 1-IP isomer) that is consistent with such a process occurring on ultrafast timescales.

Allum, Felix [Deutsches Elektronen-Synchrotron (DE↗

DOE OSTI2026

Fragmentation dynamics of CS 2 dications and trications following S 2p ionization

Here, we present the results from a detailed study of the fragmentation dynamics of CS$_2^{2+}$ and CS$_2^{3+}$, formed in intense femtosecond soft x-ray pulses above the sulfur 2p edge, primarily through single core photoionization from the S 2p site, and subsequent Auger–Meitner decay(s). By combining three-dimensional velocity map imaging with covariance analysis, we determine the relative momenta of the ions produced in each two- and three-body fragmentation channel, at significantly higher ion count rates than conventional coincidence measurements. We shed new light on the wide range of fragmentation channels observed from the CS 2 dication and trication, including channels that involve ionization-induced bond formation and fragmentations producing undetected neutral cofragments. In the latter case, a “native frames” approach is used to isolate contributions from concerted and sequential fragmentations and extract dynamical information about each step of a concerted fragmentation process. While dications often fragment sequentially, the trication is dominated by concerted fragmentation. The main trication fragmentation channel into S + + C + + S + can be well-approximated by classical Coulombic simulations of the ground-state geometry distribution, reflecting both the nature of the trication potential energy surface and the rapid multiple ionization prior to substantial structural dynamics. This study demonstrates ways in which fundamental insights into the fragmentation dynamics of polycations following x-ray ionization may be extracted, which will be beneficial to future studies that employ time-resolved x-ray Coulomb explosion imaging to study ultrafast photochemistry.

Allum, Felix [Deutsches Elektronen-Synchrotron (DE↗

DOE OSTI2025

XRISM high-resolution X-ray spectroscopy of Cygnus X-1: Highly ionized iron absorption structures

We present the first high-resolution X-ray spectral analysis of Cygnus X-1 using XRISM. The observation wa3s carried out from 2024 April 7 to 10, covering the orbital phase range 0.65–0.17 during its low/hard state. Taking advantage of the exceptional energy resolution of the Resolve instrument, we examined highly ionized iron absorption lines and characterized the ionization states, column densities, and line-of-sight velocities of the absorbing plasma. Spectral analysis revealed an ionization parameter of $\xi \sim 3$, column densities of a few $\times 10^{21}$ cm$^{-2}$, and a blueshifted velocity of $\sim$100 km s$^{-1}$. The observation was divided into two phases: before and after orbital phase $\phi _{\rm {orb}} = 0.9$, corresponding to non-dipping and dipping intervals. While only weak absorption features were present before $\phi _{\rm {orb}} = 0.9$, strong absorption by He-like and H-like Fe appeared during the dipping phase. We measured equivalent widths of 2.3, 0.4, and 1.2 eV for He-like Fe K$\alpha$ and H-like Ly$\alpha _1$ and Ly$\alpha _2$, respectively—demonstrating the capability of XRISM Resolve to securely detect narrow absorption features of only a few eV. These measurements trace the motion of the absorbing material and offer insight into the kinematics and spatial distribution of the wind in the vicinity of the black hole. These findings enhance our understanding of wind-fed accretion in Cygnus X-1 and highlight the importance of continued high-resolution X-ray observations to further constrain the physical properties of winds and accretion flows in high-mass X-ray binaries.

Astronomy and AstroPhysics↗

DOE OSTI2025

Photoelectron–residual-ion interaction in angle-resolved streaked shake-up ionization of helium

Streaked photoelectron emission spectra access the correlated dynamics of photoelectrons and residual target electrons with attosecond temporal resolution. Here, we calculated ab initio single-ionization spectra for photoemission from helium atoms by colinearly polarized ultrashort XUV and assisting few-femtosecond IR pulses. Distinguishing direct and shake-up ionization resulting in ground-state and excited (𝑛 = 2, 3) He + residual ions, respectively, we examined the effects of the correlated photoemission dynamics on the photoelectron phase accumulation as a function of the observable photoelectron detection direction and kinetic energy and XUV–IR pulse delay. We tracked the dynamical evolution of the residual ion in relative streaked photo- emission delays and found dominant contributions for shake-up emission from the residual-ion–photoelectron interaction. These are in very good and fair agreement, respectively, for 𝑛 = 2 and 𝑛 = 3 shake-up photoemission along the pulse-polarization directions, with previous experimental and theoretical investigations [Ossiander et al ., Nat. Phys. 13, 280 (2017)] and reveal a strong photoemission-direction dependence for shake-up ionization due to the coupling between the photoelectron and evolving residual-ion charge distribution in the IR-laser field.

Stark effect↗

DOE OSTI2024

Search for Dark Matter Ionization on the Night Side of Jupiter with Cassini

We present a new search for dark matter (DM) using planetary atmospheres. We point out that annihilating DM in planets can produce ionizing radiation, which can lead to excess production of ionospheric H 3 + . We apply this search strategy to the night side of Jupiter near the equator. The night side has zero solar irradiation, and low latitudes are sufficiently far from ionizing auroras, leading to a low-background search. We use data on ionospheric H 3 + emission collected three hours either side of Jovian midnight, during its flyby in 2000, and set novel constraints on the DM-nucleon scattering cross section down to about 10 − 38 cm 2 . We also highlight that DM atmospheric ionization may be detected in Jovian exoplanets using future high-precision measurements of planetary spectra. Published by the American Physical Society 2024

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2025

State selectivity in core ionization of methane

A clear experimental signature of the population of the lowest triplet state T 1 3 of the methane dication is identified in a photoionization experiment. This state is populated only in valence ionization and is absent when the dication is formed by core ionization followed by Auger-Meitner decay. For valence ionization, the total internal energy of the CH 3 + fragment, formed during the deprotonation of CH 4 2 + , is evaluated. Notably, the distribution of this internal energy peaks at the same value regardless of the initially populated electronic state of CH 4 2 + . We find that excited electronic states of CH 3 + are predominantly populated with significant rovibrational excitation. Published by the American Physical Society 2025

Rajput, J. (ORCID:0000000157752543)↗

DOE OSTI2026

Sensitivity to low-mass WIMPs with an improved liquid argon ionization response model within the DarkSide program

Dark matter detection experiments using liquid argon rely on a precise characterization of the ionization response to nuclear recoils, especially in the keV energy range relevant for light dark matter interactions. In this work, we present a comprehensive analysis that combines new measurements from the ReD setup, part of the DarkSide experimental program, with calibration data from DarkSide-50, as well as results from the ARIS and SCENE experiments. These combined datasets enable improved constraints on atomic screening effects in the modeling of the ionization response of liquid argon to nuclear recoils. The analysis is performed within the Thomas-Imel recombination framework adopted in previous DarkSide studies, and is here further constrained by the inclusion of ReD data, which allow the screening function to be determined from calibration measurements. By including the updated ionization model into the DarkSide-50 analysis framework, we obtain stronger exclusion limits on low-mass weakly interacting massive particle (WIMP) interactions, setting new world-leading constraints in the 1 – 3 GeV / c 2 WIMP mass range. Finally, we recast the sensitivity projections for the upcoming DarkSide-20k detector, demonstrating a significantly enhanced discovery potential for low-mass dark matter candidates.

Acerbi, F. [Fond. Bruno Kessler, Trento]↗

DOE OSTI2024

Quantum sensing using a qubit for the detection of ionizing radiation

Quantum sensing utilizes the inherent sensitivity of a quantum system to external stimuli. Our goal is to leverage this sensitivity to develop a quantum sensor designed for the detection of ionizing radiation. Here we report on the design, fabrication, and measurement of a new quantum device for hard x-ray and gamma-ray detection. Our quantum device is based on a superconducting quantum bit (qubit) with superconducting tunnel junctions as the core device elements. We describe our experimental investigation directed toward the detection metrics of energy resolution, dynamic range, and active area. In contrast to existing superconducting detectors, the active area per qubit may be much larger than the physical area of the tunnel junctions or the physical area of the qubit device, due to the sensitivity of quantum coherence to ionizing radiation deposition within a radius on the millimeter or centimeter scale. Furthermore, our experimental design enables an ionizing radiation source at room temperature to be detected by our quantum sensor at low temperature.

qubit↗