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DOE OSTI2024

Fine-Tuning Microporosity of Crystalline Vanadomolybdate Frameworks for Selective Adsorptive Separation of Kr from Xe

Selective adsorptive capture and separation of chemically inert krypton (Kr) and xenon (Xe) noble gases with very low ppmv concentrations in air and industrial off-gases constitute an important technological challenge. Here, using a synergistic combination of experiment and theory, the microporous crystalline vanadomolybdates (MoVO x ) as highly selective Kr sorbents are studied in detail. By varying the Mo/V ratios, we show for the first time that their one-dimensional (1D) pores can be fine-tuned for the size-selective adsorption of Kr over the larger Xe with selectivities reaching >100. Using extensive electronic structure calculations and grand canonical Monte Carlo simulations, the competition between Kr uptake with CO 2 and N 2 was also investigated. As most materials reported so far are selective toward the larger, more polarizable Xe than Kr, this work constitutes an important step toward robust Kr-selective sorbent materials. Furthermore this work highlights the potential use of porous crystalline transition metal oxides as energy-efficient and selective noble gas capture sorbents for industrial applications.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2023

Isotope study of the nonlinear pressure shifts of 85 Rb and 87 Rb hyperfine resonances in Ar, Kr, and Xe buffer gases

Measurements of the 0–0 hyperfine resonant frequencies of ground-state 85 Rb atoms show a nonlinear dependence on the pressure of the buffer gases Ar, Kr, and Xe. The nonlinearities are similar to those previously observed with 87 Rb and 133 Cs and presumed to come from alkali-metal–noble-gas van der Waals molecules. However, the shape of the nonlinearity observed for Xe conflicts with previous theory, and the nonlinearities for Ar and Kr disagree with the expected isotopic scaling of previous 87 Rb results. Improving the modeling alleviates most of these discrepancies by treating rotation quantum mechanically and considering additional spin interactions in the molecules. Including the dipolar-hyperfine interaction allows simultaneous fitting of the linear and nonlinear shifts of both 85 Rb and 87 Rb in either Ar, Kr, or Xe buffer gases with a minimal set of shared, isotope-independent parameters. To the limit of experimental accuracy, the shifts in He and N 2 were linear with pressure. Further, the results are of practical interest to vapor-cell atomic clocks and related devices.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Evolution of collectivity in 118 Xe

A recoil-distance Doppler shift experiment has been performed using the Pd 102 ( F 19 , p 2 n ) reaction at a beam energy of 73 MeV to measure the lifetime of excited states in Xe 118 . Additionally, the differential decay-curve method using γ γ coincidences and a gating procedure that allows to extract the lifetime without feeding assumptions has been employed. The lifetimes obtained for the yrast states up to spin-parity 8 + are compared with interacting boson model calculations and Xe 118 can be classified as a transitional nucleus between the spherical and a deformed shape. Systematics of the B ( E 2 ) values for the 2 + → 0 + and 4 + → 2 + transitions in the isotopic chains of tin, tellurium and xenon are presented. It is proposed that a “critical point” exists at which the B ( E 2 ; 4 + → 2 + ) / B ( E 2 ; 2 + → 0 + ) ratio drops to unity for lower neutron numbers within the isotopic chain. The position of the “critical point” varies with proton number, i.e., it is presumed to be located at the same mass number A = 114 in the Sn, Te, and Xe isotopes.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2021

Projected sensitivity of the LUX-ZEPLIN experiment to the two-neutrino and neutrinoless double $\beta$ decays of $^{134}$Xe

The projected sensitivity of the LUX-ZEPLIN (LZ) experiment to two-neutrino and neutrinoless double beta decay of 134 Xe is presented. LZ is a 10-tonne xenon time projection chamber optimized for the detection of dark matter particles, that is expected to start operating in 2021 at Sanford Underground Research Facility, USA. Its large mass of natural xenon provides an exceptional opportunity to search for the double beta decay of 134 Xe, for which xenon detectors enriched in 136 Xe are less effective. For the two-neutrino decay mode, LZ is predicted to exclude values of the half-life up to 1.7 x 10 24 years at 90% confidence level (CL), and has a three-sigma observation potential of 8.7 x 10 23 years, approaching the predictions of nuclear models. For the neutrinoless decay mode LZ, is projected to exclude values of the half-life up to 7.3 x 10 24 years at 90% CL.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2023

Lifetime measurement of excited states in 116 Xe

Lifetimes of excited states in 116 Xe were measured using the recoil-distance Doppler-shift technique. Excited 116 Xe nuclei were populated in the fusion-evaporation reaction 102 Pd( 16 O,2n) 116 Xe. Lifetimes of the $2^{+}_{1}$ and $4^{+}_{1}$ states were evaluated using the differential decay-curve method with $\gamma$-$\gamma$-coincidence data as well as lifetimes of the $6^{+}_{1}$ and $7^{-}_{1}$ states using simulations of spectra considering Doppler-shift attenuation effects.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2021

Search for double-beta decay of $$\mathrm {^{130}Te}$$ to the $$0^+$$ states of $$\mathrm {^{130}Xe}$$ with CUORE

Abstract The CUORE experiment is a large bolometric array searching for the lepton number violating neutrino-less double beta decay ( $$0\nu \beta \beta $$ 0 ν β β ) in the isotope $$\mathrm {^{130}Te}$$ 130 Te . In this work we present the latest results on two searches for the double beta decay (DBD) of $$\mathrm {^{130}Te}$$ 130 Te to the first $$0^{+}_2$$ 0 2 + excited state of $$\mathrm {^{130}Xe}$$ 130 Xe : the $$0\nu \beta \beta $$ 0 ν β β decay and the Standard Model-allowed two-neutrinos double beta decay ( $$2\nu \beta \beta $$ 2 ν β β ). Both searches are based on a 372.5 kg $$\times $$ × yr TeO $$_2$$ 2 exposure. The de-excitation gamma rays emitted by the excited Xe nucleus in the final state yield a unique signature, which can be searched for with low background by studying coincident events in two or more bolometers. The closely packed arrangement of the CUORE crystals constitutes a significant advantage in this regard. The median limit setting sensitivities at 90% Credible Interval (C.I.) of the given searches were estimated as $$\mathrm {S^{0\nu }_{1/2} = 5.6 \times 10^{24} \, \mathrm {yr}}$$ S 1 / 2 0 ν = 5.6 × 10 24 yr for the $${0\nu \beta \beta }$$ 0 ν β β decay and $$\mathrm {S^{2\nu }_{1/2} = 2.1 \times 10^{24} \, \mathrm {yr}}$$ S 1 / 2 2 ν = 2.1 × 10 24 yr for the $${2\nu \beta \beta }$$ 2 ν β β decay. No significant evidence for either of the decay modes was observed and a Bayesian lower bound at $$90\%$$ 90 % C.I. on the decay half lives is obtained as: $$\mathrm {(T_{1/2})^{0\nu }_{0^+_2} > 5.9 \times 10^{24} \, \mathrm {yr}}$$ ( T 1 / 2 ) 0 2 + 0 ν > 5.9 × 10 24 yr for the $$0\nu \beta \beta $$ 0 ν β β mode and $$\mathrm {(T_{1/2})^{2\nu }_{0^+_2} > 1.3 \times 10^{24} \, \mathrm {yr}}$$ ( T 1 / 2 ) 0 2 + 2 ν > 1.3 × 10 24 yr for the $$2\nu \beta \beta $$ 2 ν β β mode. These represent the most stringent limits on the DBD of $$^{130}$$ 130 Te to excited states and improve by a factor $$\sim 5$$ ∼ 5 the previous results on this process.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2022

Monitoring Noble Gases (Xe and Kr) and Aerosols (Cs and Rb) in a Molten Salt Reactor Surrogate Off-Gas Stream Using Laser-Induced Breakdown Spectroscopy (LIBS)

In this study with surrogate materials we show that laser-induced breakdown spectroscopy (LIBS) is a robust tool with promising capability toward monitoring gaseous (Xe and Kr) and aerosol (Cs and Rb) species in an off-gas stream from a molten salt reactor (MSR). MSRs will continually evolve fission products into the cover gas flowing across the reactor headspace. The cover gas entrains Xe and Kr gases, along with aerosol particles, before passing into an off-gas treatment system. Univariate models of Xe and Kr peaks showed a strong correlation to concentration indicated by their coefficients of determination of 0.983 and 0.997, respectively. Multivariate models were built for all four analytes using partial least squares regression coupled with preprocessing steps including normalization, trimming, and/or genetic algorithm derived filters. The models were evaluated by predicting the concentrations of the analytes in four validation samples, in which all calibration models were successfully validated at a confidence interval of 99.9%. Finally, pressure controllers were used to regulate the mass flow rate of Kr flowing into the measurement cell in sinusoidal and stepwise waveforms to test the real-time monitoring capabilities of the regression models. Both univariate and partial least squares Kr models were able to successfully quantify the gas concentration in the real-time evaluation. The root mean squared error of prediction (RMSEP) values for these real-time tests were calculated to be 0.051, 0.060, and 0.121 mol% demonstrating the measurement systems’ capability to perform online monitoring with acceptable accuracy.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2026

Accelerated 133 Xe Quantification in Samples Containing Significant 133 mXe

The quantification of 133 Xe in the presence of its mother radionuclide 133 mXe requires the full quantification of both to perform the ingrowth correction for 133 Xe. Due to the nature of both of these radionuclides, the 133 mXe requires significantly more time to quantify by High Purity Germanium (HPGe) detectors due to lower production yields, lower gamma emission probabilities, and lower detection efficiencies. This work shows that 133 Xe and 133 mXe quantification can be accelerated by measuring the 133m:133 activity ratio for a large batch of material and applying this activity ratio to assays of lower activity subsamples of the same batch of material. Included in this report are derivations of the required decay correction equations, and experiments using actual samples to validate the performance of these equations. A detector calibration method is also shown that leverages this method as an alternative to existing calibration methods for 133 mXe quantification.

133mXe↗

DOE OSTI2023

Ultrafast Laser-Excited Optical Emission of Xe under Loose-Focusing Conditions

The optical filament-based radioxenon sensing can potentially overcome the constraints of conventional detection techniques that are relevant for nuclear security applications. This study investigates the spectral signatures of pure xenon (Xe) when excited by ultrafast laser filaments at near-atmosphericpressure and in short and loose-focusing conditions. The two focusing conditions lead to laser intensity differences of several orders of magnitude and different plasma transient behavior. The gaseous sample was excited at atmospheric pressure using ∼7 mJ pulses with a 35 fs pulse duration at 800 nm wavelength. The optical signatures were studied by time-resolved spectrometry and imaging in orthogonal light collection configurations in the ∼400 nm (VIS) and ∼800 nm (NIR) spectral regions. The most prominent spectral lines of atomic Xe are observable in both focusing conditions. An on-axis light collection from an atmospheric air–Xe plasma mixture demonstrates the potential of femtosecond filamentation for the remote sensing of noble gases.

47 OTHER INSTRUMENTATION↗

DOE OSTI2020

Photoionization of Xe 5s: angular distribution and Wigner time delay in the vicinity of the second Cooper minimum

We report the angular distribution and photoionization Wigner time delay of Xe 5s photoelectrons are studied in the region of the second Cooper minimum (SCM) using (i) the relativistic multiconfiguration Tamm–Dancoff approximation, (ii) the relativistic-random-phase approximation (RRPA) and (iii) the RRPA-with-relaxation to demonstrate how differing treatments of correlation, and the relativistic interactions, affect the results. The results of the three methods are compared with each other and with available experimental data. The comparison reveals the importance of electron correlations for which a multiconfiguration description of the initial state is essential. The spin-resolved and spin-averaged photoionization time delay results show important signatures in the region of the SCM in the Xe 5s photoionization cross-section.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2025

Analysis of 127 Xe tracer measurements using a net counts method

A suite of measurement systems were deployed as part of the Physical Experiment 1 series of experiments, which involved detonating chemical explosives along with radionuclide tracers in an underground cavity, at the Nevada National Security Site (NNSS) in the United States. One of the radionuclide tracers, 127 Xe was released from the containment following the explosion and detected on a SAUNA Q B sampler situated approximately 3.5 km away. The system uses a beta-gamma coincidence detector system to measure fission product radioisotopes of xenon relevant to nuclear explosion monitoring. In this work we use the coincidence measurement data to analyse and interpret the results from the SAUNA Q B system, to calculate the measured 127 Xe activity concentration(s).

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

DOE OSTI2020

Materials Data on Xe by Materials Project

Xe is beta Polonium-like structured and crystallizes in the trigonal R-3m space group. The structure is zero-dimensional and consists of three xenon molecules. Xe is bonded in a 1-coordinate geometry to atoms.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Materials Data on Xe by Materials Project

Xe is Magnesium structured and crystallizes in the hexagonal P6_3/mmc space group. The structure is zero-dimensional and consists of two xenon molecules. Xe is bonded in a 1-coordinate geometry to atoms.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Materials Data on Xe by Materials Project

Xe is Copper structured and crystallizes in the cubic Fm-3m space group. The structure is zero-dimensional and consists of four xenon molecules. Xe is bonded in a 1-coordinate geometry to atoms.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Materials Data on Xe by Materials Project

Xe is Copper structured and crystallizes in the trigonal R-3m space group. The structure is zero-dimensional and consists of three xenon molecules. Xe is bonded in a 1-coordinate geometry to atoms.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Materials Data on Xe by Materials Project

Xe is Tungsten structured and crystallizes in the cubic Im-3m space group. The structure is zero-dimensional and consists of two xenon molecules. Xe is bonded in a 1-coordinate geometry to atoms.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Materials Data on Xe by Materials Project

Xe crystallizes in the orthorhombic Cmce space group. The structure is zero-dimensional and consists of eight xenon molecules. Xe is bonded in a 1-coordinate geometry to atoms.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Materials Data on Xe by Materials Project

Xe is alpha Samarium structured and crystallizes in the trigonal R-3m space group. The structure is zero-dimensional and consists of nine xenon molecules. Xe is bonded in a 1-coordinate geometry to atoms.

36 MATERIALS SCIENCE↗