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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 19 records

Plasma Lens in Parametric Resonance Ionization Cooling

We present a concept of a plasma lens in a parametric resonance ionization cooling (PIC) for extra cooling of muon colliders. The PIC concept has been developed to overcome most aberrations. However, parasitic non-linear aberrations which is induced in an ionization cooling material still reduce a dynamic aperture of the PIC. The plasma lens generates an azimuthally symmetric focusing field in gas-filled RF cavities that is several orders of magnitude stronger than the conventional superconducting magnets. It allows for reduction of the beam size at the beam expansion points. This reduces the size of the aberrations and therefore greatly simplifies their compensation.

43 PARTICLE ACCELERATORS↗

Developing a Th Resonance Ionization Scheme: for Future Use in Age Dating SNM by Resonance Ionization Mass Spectrometry

We report the development of a Th resonance ionization scheme (RIS) for analyzing Th isotopes by resonance ionization mass spectrometry (RIMS) to enable age-dating via the 230 Th/ 234 U inter-elemental pair. This report summarizes the work that completes the first of two tasks that are required for developing U-Th dating via RIMS at the Laser Ionization of Neutrals (LION) laboratory at Lawrence Livermore National Laboratory (LLNL). The first task involves choosing and vetting an appropriate Th RIS for the LION instrument and simultaneous U and Th analysis.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

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↗

Resonance ionization mass spectrometry for isotopic abundance measurements

Resonance ionization mass spectrometry (RIMS) is a relatively new laser-based technique for the determination of isotopic abundances. The resonance ionization process depends upon the stepwise absorption of photons from the laser, promoting atoms of the element of interest through progressively higher electronic states until an ion is formed. Sensitivity arises from the efficiency of the resonant absorption process when coupled with the power available from commercial laser sources. Selectivity derives naturally from the distinct electronic structure of different elements. This isobaric discrimination has provided the major impetus for development of the technique. Resonance ionization mass spectrometry was used for analysis of the isotopic abundances of the rare earth lutetium. Isobaric interferences from ytterbium severely effect the ability to measure small amounts of the neutron-deficient Lu isotopes by conventional mass spectrometric techniques. Resonance ionization for lutetium is performed using a continuous-wave laser operating at 452 nm, through a sequential two-photon process, with one photon exciting the intermediate resonance and the second photon causing ionization. Ion yields for microgram-sized quantities of lutetium lie between 10(6) and 10(7) ions per second, at overall ionization efficiencies approaching 10(-4). Discrimination factors against ytterbium greater than 10(6) have been measured. Resonance ionization for technetium is also being explored, again in response to an isobaric interference, molybdenum. Because of the relatively high ionization potential for Tc, three-photon, two-color RIMS processes are being developed.

Miller, C. M.↗

Development and investigation of efficient resonance ionization mass spectrometry schemes of gadolinium

Resonance ionization mass spectrometry of gadolinium can be used for nuclear forensics and to further the understanding of stellar nucleosynthesis but has been used only a handful of times due to the high laser power required and interference from non-resonant ionization of molecules of other elements. Herein we present the development of two novel resonance ionization spectroscopy schemes for gadolinium that provide improvements in isotopic fractionation and ionization efficiency, respectively, opening new applications for gadolinium analysis. The schemes are demonstrated and compared in a mixed sample of gadolinium and neodymium.

and nuclear chemistry↗

Resonance ionization of zirconium

Abstract Measuring the isotopic composition of trace Zr in presolar stardust grains allows us to study the environment of slow neutron-capture nucleosynthesis in asymptotic giant branch stars. Here, we present a newly characterized Zr resonance ionization scheme that can be saturated with state-of-the-art titanium-sapphire lasers and yields a useful yield of (5.4 ± 0.4)%. Resonance ionization is achieved in two steps: after first being excited with a photon at 319.215 nm, neutral Zr atoms are then ionized with a photon at 388.988 nm, where both wavelengths are reported as in vacuum.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

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↗

Voltage scanning and technical upgrades at the Collinear Resonance Ionization Spectroscopy experiment

To optimize the performance of the Collinear Resonance Ionization Spectroscopy (CRIS) experiment at CERN-ISOLDE, technical upgrades are continuously introduced, aiming to enhance its sensitivity, precision, stability, and efficiency. Recently, a voltage-scanning setup was developed and commissioned at CRIS, which improved the scanning speed by a factor of three as compared to the current laser-frequency scanning approach. This leads to faster measurements of the hyperfine structure for systems with high yields (more than a few thousand ions per second). Additionally, several beamline sections have been redesigned and manufactured, including a new field-ionization unit, an electrostatic bend with a larger deflection angle, and improved ion optics. The beamline upgrades are expected to yield an improvement of at least a factor of 5 in the signal-to-noise ratio by avoiding the use of high-power lasers (which yield non-resonantly produced ions) and providing time-of-flight separation between the resonant ions and the collisional background.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

High efficiency laser resonance ionization of plutonium

Three-step resonance photoionization spectra of plutonium have been studied with Ti:Sapphire lasers for the development of efficient laser ionization schemes for ultra-trace analysis of Pu isotopes by resonance ionization mass spectrometry. We observed eighteen intermediate excited states of even parity in the energy range 35568–36701 cm -1 , thirteen of them have not been previously documented, and a larger number of high-lying excited states and autoionizing states of odd-parity between 48238 and 49510 cm -1 . Three-color, three-photon ionization schemes via six intermediate states were evaluated under similar ion source operating conditions. This led to a highly efficient three-step scheme with an overall ionization efficiency of 51.1±1.3%, which is an order of magnitude improvement over the previously reported ionization efficiency for Pu.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

One-dimensional temperature measurement of supersonic jet flow by resonantly ionized photoemission thermometry of molecular nitrogen

As the field of fluid dynamics progresses, the demand for sophisticated diagnostic methods to accurately assess flow conditions rises. In this work, resonantly ionized photoemission thermometry (RIPT) has been used to directly target and ionize diatomic nitrogen (N 2 ) to measure one-dimensional (1D) temperature profiles in a supersonic jet flow. This technique can be considered non-intrusive as the premise uses resonantly enhanced multiphoton ionization (REMPI) to target molecular nitrogen. This resonance excites N 2 into absorption bands of the P, Q, and R rotational branches of N 2 ( b 1 Π u ). The ideal (3 + 1) REMPI scheme excites from the ground state and ionizes N 2 ( b 1 Π u ← X 1 Σ g + ) where de-excitation results in photoemission from the first negative band of ionized N 2 + ( B 2 Σ u + → X 2 Σ g + ) as nitrogen returns to the ground state. The resulting emission can be observed using an intensified camera, thus permitting inference of the rotational temperature of ground-state molecular nitrogen. A linearly regressive Boltzmann distribution is applied based on previous calibration data for this technique to quantify the temperature along the ionized line. This work applies this technique to a pure N 2 supersonic jet in cross-flow and counter-flow orientations to demonstrate N 2 RIPT’s applications in a supersonic flow. Temperature variations are observed at different locations downstream of the exit in cross-flow, and axisymmetric in counter-flow, to generate profiles characterizing the flow dynamics. Due to the collisional effects resulting from the number density of N 2 at higher pressures, a (3 + 2) REMPI scheme is observed throughout this text.

Clark, Aleksander (ORCID:0009000855600042)↗

Simultaneous Isotopic Analysis of U, Pu, and Am in Spent Nuclear Fuel by Resonance Ionization Mass Spectrometry

Solid samples of spent nuclear fuel were analyzed for actinide isotopic composition by resonance ionization mass spectrometry. Isotopes of U, Pu, and Am were simultaneously quantified using a new method that removes and/or resolves the isobaric interferences at 238 U/ 238 Pu and 241 Pu/ 241 Am without sample preparation other than cutting and mounting small (~10 μm) samples. Trends in burnup and neutron capture product distributions were correlated with the sampling positions inside the reactor. Overall, the results show the skin effect, in which the core and near-edge regions of a fuel pellet exhibit strong differences in actinide concentrations and isotope distributions due to differences in the neutron energy spectra between the pellet rim and the core. While no elemental concentration measurements were made, the ability to measure the 238 Pu/ 239 Pu ratio in the presence of a 7400× excess of 238 U enabled an estimate of the enhancement in Pu concentration due to the skin effect at the rim of the pellet.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Nonseeded linewise temperature measurements by resonantly ionized photoemission thermometry in a Mach 4 Ludwieg tube

A one-dimensional (1D) thermometry using oxygen-tagging resonantly ionized photoelectron thermometry (O 2 RIPT) was employed to investigate thermal gradients within a Mach 4 Ludwieg tube. The Ludwieg tube is pulsed with a test duration of approximately 100 ms, providing a cold supersonic flow at Mach 4 ideal for studying aerothermal effects. This study focused on measuring freestream temperatures, capturing shock-induced heating behind a detached bow shock from a blunt cylinder, and resolving sharp temperature variations across a bow shock generated by a cylinder. The O 2 RIPT technique produced strong emission signals extending approximately 4 cm long, demonstrating its capability for precise temperature measurements in high-speed wind tunnel environments. The results confirm that O 2 RIPT is well-suited for applications in large-scale aerodynamic testing facilities, particularly in regions with strong compression effects, enabling the resolution of sharp thermal gradients. This method presents a promising solution for thermometry in dynamic flow conditions relevant to various experimental ground-test facilities.

McCord, Walker (ORCID:0000000179747550)↗

Simultaneous isotopic analysis of fission product Sr, Mo, and Ru in spent nuclear fuel particles by resonance ionization mass spectrometry

Abstract Fission product Sr, Mo, and Ru isotopes in six 10-μm particles of spent fuel from a pressurized water reactor were analyzed by resonance ionization mass spectrometry (RIMS) and evaluated for utility in nuclear material characterization. Previous measurements on these same samples showed widely varying U, Pu, and Am isotopic compositions owing to the samples’ differing irradiation environments within the reactor. This is also seen in Mo and Ru isotopes, which have the added complication of exsolution from the UO 2 fuel matrix. This variability is a hindrance to interpreting data from a collection of particles with incomplete provenance since it is not always possible to assign particles to the same batch of fuel based on isotopic analyses alone. In contrast, the measured 90 Sr/ 88 Sr ratios were indistinguishable across all samples. Strontium isotopic analysis can therefore be used to connect samples with otherwise disparate isotopic compositions, allowing them to be grouped appropriately for interpretation. Strontium isotopic analysis also provides a robust chronometer for determining the time since fuel irradiation. Because of the very high sensitivity of RIMS, only a small fraction of material in each of the 10 μm samples was consumed, leaving the vast majority still available for other analyses.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Laser resonance ionization spectroscopy of thorium

High-lying Rydberg and autoionizing (AI) states of thorium (Th) have been studied via resonance laser ionization spectroscopy at both TRIUMF Canada’s particle accelerator center and Oak Ridge National Lab (ORNL). Multiple Rydberg series converging to the ionization potential (IP) were observed via different stepwise laser excitation schemes and were assigned to be the 6d 2 7s ( 4 F 3/2 ) np, nd, and nf series. Analysis of these series enabled the determination of the IP to be 50 868.735(54) cm −1 , which improved the precision by two orders of magnitude over the current adopted NIST value of 50 867(2) cm −1 . Additionally, four AI Rydberg series were identified and assigned to nf and nd series converging to the 6d 2 7s 4 F 5/2 and 6d7s 2 2 D 3/2 metastable states of Th + . In conclusion, the measured energies of the Rydberg and AI Rydberg states are reported, and observed perturbations within the series are discussed.

Rydberg series↗

O 2 based resonantly ionized photoemission thermometry analysis of supersonic flows

Characterization of the thermal gradients within supersonic and hypersonic flows is essential for understanding transition, turbulence, and aerodynamic heating. Developments in novel, impactful non-intrusive techniques are key for enabling flow characterizations of sufficient detail that provide experimental validation datasets for computational simulations. In this work, Resonantly Ionized Photoemission Thermometry (RIPT) signals are directly imaged using an ICCD camera to realize the techniques 1D measurement capability for the first time. The direct imaging scheme presented for oxygen-based RIPT (O 2 RIPT) uses the previously established calibration data to direct excite various resonant rotational peaks within the S-branch of the C 3 Π, ( v = 2) ← X 3 Σ( v ′ = 0) absorption band of O 2 . The efficient ionization of O 2 liberates electrons that induce electron avalanche ionization of local N 2 molecules generating N 2 + , which primarily deexcites via photoemissions of the first negative band of N 2 + ( B 2 Σ <#comment/> u + − <#comment/> X 2 Σ <#comment/> g + ) . When sufficient lasing energy is used, the ionization region and subsequent photoemission signal is achieved along a 1D line thus, if directly imaged can allow for gas temperature assignments along said line; demonstrated here of up to five centimeters in length. The temperature gradients present within the ensuing shock train of a supersonic under expanded free jet serves as a basis of characterization for this new RIPT imaging scheme. The O 2 RIPT results are extensively compared and validated against well-known and established techniques (i.e., CARS and CFD). The direct imaging capability fully realizes the technique’s fundamental potential and is expected to be the standard of implementation going forward. The direct imaging capability can play instrumental roles in future scientific studies that rely upon acute characterization of thermal gradients within a medium that cannot be easily resolved by a point. Furthermore, the removal of the spectrometer greatly reduces the cost, complexity, and optical alignment associated with prior RIPT measurements.

42 ENGINEERING↗