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All sourcesNASA NTRSDOE OSTI
DOE OSTI2011

Nuclear Data Sheets for A = 44

The experimental data are evaluated for known nuclides of mass number A=44 (Si,P,S,Cl,Ar,K,Ca,Sc,Ti,V, Cr,Mn). Detailed evaluated level properties and related information are presented, including adopted values of level and {gamma}-ray energies, decay data (energies, intensities and placement of radiations), and other spectroscopic data. This work supersedes earlier full evaluations of A=44 published by 1999Ca45 and 1990En08 (also 1998En04 update). No excited states are known in {sup 44}Si, {sup 44}P, {sup 44}Cr, {sup 44}Mn. Only one excited state is known in 44V and its Isobaric Analog State (IAS) has been observed but with the level energy not known. Information for {sup 44}S, {sup 44}Cl and {sup 44}Ar is limited and their radioactive decay schemes seem incomplete in view of large Q values and known excitations much below than allowed by Q values. The {sup 44}Ca, {sup 44}Sc and {sup 44}Ti nuclides remain as the most extensively studied from many different reactions and decays.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2011

The ground state g factor of {sup 44}Cl : a probe for the reduced gaps at Z 16 and N = 28

The g factor of the {sup 44}Cl ground state is measured at the LISE fragment separator at the Grand Accelerateur National d'Ions Lourds (GANIL) using the {beta} nuclear magnetic resonance technique, resulting in g({sup 44}Cl) (-)0.2749(2). An analysis of the g factor value and of the theoretical level scheme in the shell-model framework reveals the presence of odd-proton s{sub 1/2} configurations and neutron excitation across the N = 28 shell gap in the {sup 44}Cl ground state. In addition, the measured g factor strongly supports a 2{sup -} spin assignment for the {sup 44}Cl ground state.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2022

Molecular dynamics study of silicon atomic layer etching by chlorine gas and argon ions

Classical molecular dynamics (MD) is used to simulate atomic layer etching processes of silicon by alternating exposure to chlorine gas and argon ions. In order to validate our model, a rigorous comparison is done with ion beam experiments found in the literature [Park et al., Jpn. J. Appl. Phys. 44, 389 (2005)]. Here it is shown that the etch per cycle (EPC) as a function of argon ion energy from simulations is in quantitative agreement with experimental results if the correct argon ion fluence is used in the simulations. The EPC as a function of ion irradiation time and amount of chlorine exposure also show good agreement with the experiment. The MD simulations also show the formation of an amorphous silicon region with chlorine atoms mixed uniformly throughout following ion bombardment. Finally, the etch products during the ion irradiation step are analyzed and discussed.

74 ATOMIC AND MOLECULAR PHYSICS↗
NASA NTRSDate not supplied

Gaseous By-Product of Thermal Vacuum Processing of Lunar Highland Simulant

Scientists at Kennedy Space Center are advancing technologies to achieve oxygen extraction on the Lunar surface. One such technology is Molten Regolith Electrolysis (MRE) in which regolith simulant is melted under high temperatures to perform oxygen extraction through electrolysis of the melt pool. A study was conducted to understand the molten formation and proper-ties of Lunar Highlands Simulants (LHS-1) under high vacuum environments ranging between 10-6 Torr. These studies include investigating the regolith melt behavior and by-product gas analysis systems to prepare for pilot plant development and operations. The off-gassing rates and pressure build-up, gaseous compounds, and material compatibility may be a risk to MRE systems. The KSC findings are reported here for inclusion into future mis-sion architecture and operational planning. The four stages of the experiment were vacuum, resistive heating, regolith melt and gas detection. The regolith mass of 70 g was melted in a 40 cm tall x 50 cm diameter vacuum chamber at temperature increase rate 47 ℃ /min and ramp rate of 1 ampere/3 min up to an 18-amp maximum. The test is conducted for about 60 minutes and the constituent gases produced during heating of regolith is monitored with a re-sidual gas analyzer. During the molten formation, primary off-gassing volatiles included water vapor (18 amu), a peak at 44 amu (FeO2 – expected), and atomic oxygen (16 amu), among a series of other compounds that could create compatibility issues such as magnesium, chlorine, and silicon oxide. These results add to the knowledge required for successful oxygen extraction on the moon.

Molten Regolith Electrolysis↗
NASA NTRS2010

Thermal Properties of Lunar Regolith Simulants

Various high temperature chemical processes have been developed to extract oxygen and metals from lunar regolith. These processes are tested using terrestrial analogues of the regolith. But all practical terrestrial analogs contain H2O and/or OH(-), the presence of which has substantial impact on important system behaviors. We have undertaken studies of lunar regolith simulants to determine the limits of the simulants to validate key components for human survivability during sustained presence on the moon. Differential Thermal Analysis (DTA) yields information on phase transitions and melting temperatures. Themo-Gravimetric Analysis (TGA) with mass spectrometric (MS) determination of evolved gas species yields chemical information on various oxygenated volatiles (water, carbon dioxide, sulfur oxides, nitrogen oxides and phosphorus oxides) and their evolution temperature profiles. The DTA and TGAMS studies included JSC-1A fine, NU-LHT-2M and its proposed feed stocks: anorthosite; dunite; HQ (high quality) glass and the norite from which HQ glass is produced. Fig 1 is a data profile for anorthosite. The DTA (Fig 1a) indicates exothermic transitions at 355 and 490 C and endothermic transitions at 970 and 1235 C. Below the 355 C transition, water (Molecular Weight, MW, 18 in Fig 1c) is lost accounting for approximately 0.1% mass loss due to water removal (Fig 1b). Just above 490 C a second type of water is lost, presumably bound in lattices of secondary minerals. Between 490 and the 970 transition other volatile oxides are lost including those of hydrogen (third water type), carbon (MW = 44), sulfur (MW = 64 and 80), nitrogen (MW 30 and 46) and possibly phosphorus (MW = 79, 95 or 142). Peaks at MW = 35 and 19 may be attributable to loss of chlorine and fluorine respectively. Negative peaks in the NO (MW = 30) and oxygen (MW = 32) MS profiles may indicate the production of NO2 (MW = 46). Because so many compounds are volatilized in this temperature range quantification of the mass loss associated with individual species is difficult. Similar information will be presented for the other materials studied in this investigation.

Street, Kenneth↗
NASA NTRS2010

Thermal Properties of Lunar Regolith Simulants

Various high temperature chemical processes have been developed to extract oxygen and metals from lunar regolith. These processes are tested using terrestrial analogues of the regolith. But all practical terrestrial analogs contain H2O and/or OH-, the presence of which has substantial impact on important system behaviors. We have undertaken studies of lunar regolith simulants to determine the limits of the simulants to validate key components for human survivability during sustained presence on the moon. Differential Thermal Analysis (DTA) yields information on phase transitions and melting temperatures. Themo-Gravimetric Analysis (TGA) with mass spectrometric (MS) determination of evolved gas species yields chemical information on various oxygenated volatiles (water, carbon dioxide, sulfur oxides, nitrogen oxides and phosphorus oxides) and their evolution temperature profiles. The DTA and TGAMS studies included JSC-1A fine, NU-LHT-2M and its proposed feed stocks: anorthosite; dunite; HQ (high quality) glass and the norite from which HQ glass is produced. Fig 1 is a data profile for anorthosite. The DTA (Fig 1a) indicates exothermic transitions at 355 and 490 C and endothermic transitions at 970 and 1235 C. Below the 355 C transition, water (Molecular Weight, MW, 18 in Fig 1c) is lost accounting for approximately 0.1% mass loss due to water removal (Fig 1b). Just above 490 C a second type of water is lost, presumably bound in lattices of secondary minerals. Between 490 and the 970 transition other volatile oxides are lost including those of hydrogen (third water type), carbon (MW = 44), sulfur (MW = 64 and 80), nitrogen (MW 30 and 46) and possibly phosphorus (MW = 79, 95 or 142). Peaks at MW = 35 and 19 may be attributable to loss of chlorine and fluorine respectively. Negative peaks in the NO (MW = 30) and oxygen (MW = 32) MS profiles may indicate the production of NO2 (MW = 46). Because so many compounds are volatilized in this temperature range quantification of the mass loss associated with individual species is difficult. Similar information will be presented for the other materials studied in this investigation.

Street, Kenneth↗
DOE OSTI2022

Synthesis and characterization of uranium trichloride in alkali-metal chloride media

Given a growing interest in uranium salts for pyrochemical processing of used fuel and uranium-fueled molten salt reactors, the synthesis of uranium trichloride in alkali-metal chloride media was investigated in a series of four experiments. Specifically, uranium metal powder and uranium hydride powder were prepared and separately blended with ammonium chloride and lithium chloride – potassium chloride eutectic in two runs, while the same powders were separately blended with ammonium chloride and sodium chloride in two additional runs. Each of the lithium chloride – potassium chloride containing blends was slowly heated to 923 K, while those containing sodium chloride were heated to 1123 K. During each heat up, the ammonium chloride sublimed into gaseous ammonia and hydrogen chloride, leading to the chlorination of uranium metal or uranium hydride and the formation of molten salt solutions of the respective chlorides. Experimental conditions were incorporated in the runs to promote formation of uranium trichloride over uranium tetrachloride in the respective media. Molten samples of each run product were taken and characterized via chemical analyses, diffractometry, and microscopy. The final products from each run were dark dense ingots of the respective salt systems with uranium concentrations ranging from 44 to 51 wt%. Finally, chemical analyses and diffractometry identified the predominant presence of uranium trichloride in these systems; however, a possible minor presence of uranium tetrachloride could not be conclusively dismissed.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2012

Nitrate Conversion of HB-Line Reillex™ HPQ Resin

Reillex™ HPQ ion exchange resin is used by HB Line to remove plutonium from aqueous streams. Reillex™ HPQ resin currently available from Vertellus Specialties LLC is a chloride ionic form, which can cause stress corrosion cracking in stainless steels. Therefore, HB Line Engineering requested that Savannah River National Laboratory (SRNL) convert resin from chloride form to nitrate form in the Engineering Development Laboratory (EDL). To perform this task, SRNL treated two batches of resin in 2012. The first batch of resin from Reilly Industries Batch 80302MA was initially treated at SRNL in 2001 to remove chloride. This batch of resin, nominally 30 liters, has been stored wet in carboys since that time until being retreated in 2012. The second batch of resin from Batch 23408 consisted of 50 kg of new resin purchased from Vertellus Specialties in 2012. Both batches were treated in a column designed to convert resin using downflow of 1.0 M sodium nitrate solution through the resin bed followed by rinsing with deionized water. Both batches were analyzed for chloride concentration, before and after treatment, using Neutron Activation Analysis (NAA). The resin specification [Werling, 2003] states the total chlorine and chloride concentration shall be less than 250 ppm. The resin condition for measuring this concentration is not specified; however, in service the resin would always be fully wet. Measurements in SRNL showed that changing from oven dry resin to fully wet resin, with liquid in the particle interstices but no supernatant, increases the total weight by a factor of at least three. Therefore, concentration of chlorine or chloride expressed as parts per million (ppm) decreases by a factor of three. Therefore, SRNL recommends measuring chlorine concentration on an oven dry basis, then dividing by three to estimate chloride concentration in the fully wet condition. Chloride concentration in the first batch (No.80302MA) was nearly the same before the current treatment (759 ppm dry) and after treatment (745 ppm dry or ~248 ppm wet). Treatment of the second batch of resin (No.23408) was very successful. Chloride concentration decreased from 120,000 ppm dry to an average of 44 ppm dry or ~15ppm wet, which easily passes the 250 ppm wet criterion. Per guidance from HB Line Engineering, SRNL blended Batch 80302 resin with Batch P9059 resin which had been treated previously by ResinTech to remove chloride. The chloride concentrations for the two drums of Batch P9059 were 248 ppm dry (~83 ppm wet) ±22.8% and 583 ppm dry (~194 ppm wet) ± 11.8%. The blended resin was packaged in five gallon buckets.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
NASA NTRS1997

Balloon-Borne Measurements of Stratospheric Radicals and their Precursors: Implications for the Production and Loss of Ozone

Measurements of hydrogen, nitrogen and chlorine radicals from a balloon flight on 25 September 1993 from Ft. Sumner, NM provide an opportunity to quantify photochemical production and loss of stratospheric ozone. Ozone loss rates determined using measured radical concentrations agree fairly well with loss rates calculated using a photochemical model. Catalytic cycles involving OH and HO2 are shown to dominate photochemical loss of ozone for altitudes between 44 and 50 km. Reactions involving NO and NO2 are the dominant sink for ozone between 25 and 38 km. The total ozone loss rate determined from the measurements balances calculated production rates for altitudes between 30 and 40 km. However, loss of ozone exceeds production by -35% between 42 and 50 km. The imbalance between production and loss of ozone above 42 km is larger than the uncertainty of any one of the critical kinetic parameters or species concentrations. No single adjustment to any of these parameters can simultaneously resolve the imbalance and satisfy constraints imposed by measured OH, HO2, NO2 and ClO. Our results are consistent with an additional mechanism for ozone production above 40 km other than photolysis of ground state O2.

Osterman, G. B.↗
DOE OSTI2025

Synthesis and characterization of uranium trichloride in alkali-metal chloride media

Given a growing interest in uranium salts for pyrochemical processing of used fuel and uranium-fueled molten salt reactors, the synthesis of uranium trichloride in alkali-metal chloride media was investigated in a series of four experiments. Specifically, uranium metal powder and uranium hydride powder were prepared and separately blended with ammonium chloride and lithium chloride – potassium chloride eutectic in two runs, while the same powders were separately blended with ammonium chloride and sodium chloride in two additional runs. Each of the lithium chloride – potassium chloride containing blends was slowly heated to 923 K, while those containing sodium chloride were heated to 1123 K. During each heat up, the ammonium chloride sublimed into gaseous ammonia and hydrogen chloride, leading to the chlorination of uranium metal or uranium hydride and the formation of molten salt solutions of the respective chlorides. Experimental conditions were incorporated in the runs to promote formation of uranium trichloride over uranium tetrachloride in the respective media. Molten samples of each run product were taken and characterized via chemical analyses, diffractometry, and microscopy. The final products from each run were dark dense ingots of the respective salt systems with uranium concentrations ranging from 44 to 51 wt%. Chemical analyses and diffractometry identified the predominant presence of uranium trichloride in these systems; however, a possible minor presence of uranium tetrachloride could not be conclusively dismissed.

D Herrmann, Steven↗
DOE OSTI2024

Sustainable and Energy-Efficient Production of Rare-Earth Metals via Chloride-Based Molten Salt Electrolysis

Neodymium metal is a critical component of rare earth magnets, essential for electric vehicles and the green energy transition, but its production has severe environmental impacts across its mining, separation, purification, and metal electrowinning steps. Specifically, conventional neodymium electrowinning in oxyfluoride molten salts using a consumable graphite anode generates greenhouse gases, e.g., carbon dioxide and perfluorocarbon (PFC). We propose an alternative chloride-based molten salt electrolysis process utilizing a novel dimensionally stable anode (DSA). Our process lowers the specific electrical energy consumption compared to the state of the art, while producing reusable chlorine gas and eliminating direct CO 2 and PFC emissions. Chloride-based molten salt electrolysis of NdCl 3 (1.65 M) added to a LiCl–KCl eutectic (45:55 wt %), while using a RuO 2 -coated DSA enables high Coulombic efficiency (>80%), low specific energy consumption (2.3 kWh/kg-Nd), and excellent electrowon Nd product purity (>97 wt %). Life cycle analysis, excluding the common input feedstock (Nd 2 O 3 ), shows that the global warming potential for the proposed chloride-based electrolysis approach is 5 kg CO 2 equivalent, compared to 9–16 kg CO 2 equivalent for the conventional process, representing a 44–69% reduction in CO 2 emissions.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Quadrupole collectivity in the neutron-rich sulfur isotopes 38,40,42,44 S

Electromagnetic transition strengths in the even-even neutron-rich sulfur isotopes 38,40,42,44 S were measured using intermediate-energy Coulomb excitation at the National Superconducting Cyclotron Laboratory. By utilizing the sensitivity of the experimental technique to E2 excitations from the ground state, the evolution of the pattern of B(E2) strengths to several low-lying 2 + states was investigated at Z = 16 from near stability to the N = 28 island of inversion. The experimental results allowed a detailed comparison with predictions from shell-model calculations using the SDPF-MU Hamiltonian, which was designed to describe collectivity in this region of the nuclear chart. While the shell-model calculations succeeded in modeling transition strengths at N = 22, 24, 26, the experimental B(E2; $0$ $^{+}_{1}$ → $2$ $^{+}_{1}$) at N = 28 was smaller than the predicted value by about a factor of 2, similar to previous observations for chlorine and argon isotopes around N = 28. The dependence of this overprediction by theory on the choice of effective charges was explored.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2014

Energy levels, radiative rates, and lifetimes for transitions in W LVIII

Energy levels and radiative rates are reported for transitions in Cl-like W LVIII. Configuration interaction (CI) has been included among 44 configurations (generating 4978 levels) over a wide energy range up to 363 Ryd, and the general-purpose relativistic atomic structure package (GRASP) adopted for the calculations. Since no other results of comparable complexity are available, calculations have also been performed with the flexible atomic code (FAC), which help in assessing the accuracy of our results. Energies are listed for the lowest 400 levels (with energies up to ∼98 Ryd), which mainly belong to the 3s{sup 2}3p{sup 5}, 3s3p{sup 6}, 3s{sup 2}3p{sup 4}3d, 3s{sup 2}3p{sup 3}3d{sup 2}, 3s3p{sup 4}3d{sup 2}, 3s{sup 2}3p{sup 2}3d{sup 3}, and 3p{sup 6}3d configurations, and radiative rates are provided for four types of transitions, i.e. E1, E2, M1, and M2. Our energy levels are assessed to be accurate to better than 0.5%, whereas radiative rates (and lifetimes) should be accurate to better than 20% for a majority of the strong transitions.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2011

Effect of fresh green waste and green waste compost on mineral nitrogen, nitrous oxide and carbon dioxide from a Vertisol

Incorporation of organic waste amendments to a horticultural soil, prior to expected risk periods, could immobilise mineral N, ultimately reducing nitrogen (N) losses as nitrous oxide (N{sub 2}O) and leaching. Two organic waste amendments were selected, a fresh green waste (FGW) and green waste compost (GWC) as they had suitable biochemical attributes to initiate N immobilisation into the microbial biomass and organic N forms. These characteristics include a high C:N ratio (FGW 44:1, GWC 35:1), low total N (<1%), and high lignin content (>14%). Both products were applied at 3 t C/ha to a high N (plus N fertiliser) or low N (no fertiliser addition) Vertisol soil in PVC columns. Cumulative N{sub 2}O production over the 28 day incubation from the control soil was 1.5 mg/N{sub 2}O/m{sup 2}, and 11 mg/N{sub 2}O/m{sup 2} from the control + N. The N{sub 2}O emission decreased with GWC addition (P < 0.05) for the high N soil, reducing cumulative N{sub 2}O emissions by 38% by the conclusion of the incubation. Analysis of mineral N concentrations at 7, 14 and 28 days identified that both FGW and GWC induced microbial immobilisation of N in the first 7 days of incubation regardless of whether the soil environment was initially high or low in N; with the FGW immobilising up to 30% of available N. It is likely that the reduced mineral N due to N immobilisation led to a reduced substrate for N{sub 2}O production during the first week of the trial, when soil N{sub 2}O emissions peaked. An additional finding was that FGW + N did not decrease cumulative N{sub 2}O emissions compared to the control + N, potentially due to the fact that it stimulated microbial respiration resulting in anaerobic micro sites in the soil and ultimately N{sub 2}O production via denitrification. Therefore, both materials could be used as post harvest amendments in horticulture to minimise N loss through nitrate-N leaching in the risk periods between crop rotations. The mature GWC has potential to reduce N{sub 2}O, an important greenhouse gas.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2014

Observation of 23 supernovae that exploded <300 pc from Earth during the past 300 kyr

Four supernovae (SNe), exploding ≤300 pc from Earth, were recorded 44, 37, 32, and 22 kyr ago in the radiocarbon ({sup 14}C) record during the past 50 kyr. Each SN left a nearly identical signature in the record, beginning with an initial sudden increase in atmospheric radiocarbon, when the SN exploded, followed by a hiatus of 1500 yr, and concluding with a sustained 2000 yr increase in global radiocarbon due to γ-rays produced by diffusive shock in the SN remnant (SNR). For the past 18 kyr excess radiocarbon has decayed with the {sup 14}C half-life. SN22kyrBP, is identified as the Vela SN that exploded 250 ± 30 pc from Earth. These SN are confirmed in the {sup 10}Be, {sup 26}Al, {sup 36}Cl, and NO{sub 3}{sup −} geologic records. The rate of near-Earth SNe is consistent with the observed rate of historical SNe giving a galactic rate of 14 ± 3 kyr{sup –1} assuming the Chandra Galactic Catalog SNR distribution. The Earth has been used as a calorimeter to determine that ≈2 × 10{sup 49} erg were released as γ-rays at the time of each SN explosion and ≈10{sup 50} erg in γ-rays following each SN. The background rate of {sup 14}C production by cosmic rays has been determined as 1.61 atoms cm{sup –2} s{sup –1}. Approximately 1/3 of the cosmic ray energy produced by diffusive shock in the SNR was observed to be emitted as high-energy γ-rays. Analysis of the {sup 10}Be/{sup 9}Be ratio in marine sediment identified 19 additional near-Earth SNe that exploded 50-300 kyr ago. Comparison of the radiocarbon record with global temperature variations indicated that each SN explosion is correlated with a concurrent global warming of ≈3°C-4°C.

79 ASTRONOMY AND ASTROPHYSICS↗