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Spectral broadening of europium ions in glass
Spectral broadening mechanisms for trivalent Eu ions in glass, considering fluorescence and absorption spectra measurements
On the abundance of Europium
The inclusion of the effects of hyperfine splitting can significantly lower the abundance estimate of Eu from singly ionized lines which lie on the flat portion of the curve of growth. In the 21 cool Ap stars studied by Adelman and the five Am stars studied by Smith, the Eu abundance was reduced by 0.4 dex on the average. In individual cases, the reductions were as great as 0.9 dex. This makes the Eu abundance comparable to that of its neighboring rare earths Sm and Gd in the Ap stars and less than Sm and Gd in the Am stars, but still substantially overabundant with respect to solar values.
EPR measurement of the effect of glass composition on the oxidation states of europium
An investigation was conducted concerning the dependence of the concentration ratio of Eu(2+) to Eu(3+) on composition for silicate liquids whose compositional end members are CaAl2Si2O8 and MgSiO3, MG2SiO4, CaMgSi2O6, CaMgSiO4, CaSiO3, or Ca2SiO4. The liquids were quenched to produce glasses. An electron paramagnetic resonance spectrometer was used to determine the concentration ratios of Eu(2+) to Eu(3+) in the glasses.
Measurement of the effects of temperature and partial pressure of oxygen on the oxidation states of europium in silicate glasses
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The oxidation state of europium as an indicator of oxygen fugacity
Empirical oxygen barometers based on Eu(2+)/Eu(3+) ratios in plagioclase feldspar and magmatic liquid were developed using Philpott's (1970) approach and the experimental data of Drake (1972). Oxygen fugacities calculated on the basis of Eu(2+)/Eu(3+) ratios for terrestrial basalts cluster tightly around 10 to the negative seventh power. Oxygen fugacities for Apollo 11 and 12 lunar ferrobasalts cluster tightly around 10 to the negative 12.7 power. Calculated oxygen fugacities for achondritic meteorites are lower than for lunar samples by several orders of magnitude.
Europium mass balance in polymict samples and implications for plutonic rocks of the lunar crust
The mean concentrations of Sm and Eu in the lunar surface crust were analyzed by correlating the Sm concentration and the Sm/Eu ratio with Th concentration obtained from published data on a large number of polymict samples from various locations in the lunar highlands, and using the value of 0.91 microg/g for the mean Th concentration of the highlands surface crust obtained by the orbiting gamma-ray experiments. The mean concentration of Sm in the lunar surface crust was found to be between 2 and 3 microg/g, and that of Eu between 0.7 and 1.2 microg/g. The results indicate that there is no significant enrichment or depletion of Eu, compared to Sm, relative to chondritic abundances; i.e., there is no significant 'Eu anomaly' in average upper crust, contrary to predictions by some earlier investigators.
Europium anomalies in mare basalts as a consequence of mafic cumulate fractionation from an initial lunar magma
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Optical fiber spectroscopy: A study of the luminescent properties of the europium ion for thermal sensors
Recently, there has been interest in developing a distributed temperature sensor integrated into an optical fiber. Such a system would allow embedding of the optical fiber within or on a structural material to provide for continuous monitoring of the material's temperature. Work has already begun on the development of a temperature sensor using the temperature dependent emission spectra from the lanthanide rare earths doped into crystalline hosts. The lifetime, the linewidth and the integrated intensity of this emission are each sensitive to changes in the temperature and can provide a basis for thermometry. One concept for incorporating this phenomena into an optical fiber based sensor involves bonding the optically active material to the cladding of an optical fiber and allowing the luminescent light to couple into the the fiber by the evanescent wave. Experimental work developing this concept has already been reported. Measurements of the linewidth of Eu3+:Y2O3, diffused into a fiber, made by Albin clearly show a strong and regular dependence on temperature over the range of 300 to 1000 K. We report here on a study of the temperature dependence of the lineshape of the emission at 611 nm using the data in references. We focus attention on understanding the general behavior of the Eu3+:Y2O3 system. Building upon understanding of this system we will be able to establish the physical criterial for a good optical fiber based temperature sensor and then to examine available data on other lanthanide rare earths and transition metal ions to determine the best luminescent system for temperature sensing in an optical fiber.
Oxygen Fugacity of the Martian Mantle from Pigeonite/Melt Partitioning of Samarium, Europium and Gadolinium
This study is part of an ongoing effort to calibrate the pyroxene/melt REE oxybarometer for conditions relevant to the martian meteorites. These efforts have been motivated by reports of redox variations among the shergottites . We have conducted experiments on martian composition pigeonite/melt rare earth element partitioning as a function of fO2.
Oxygen Fugacity of the Martian Mantle from Pigeonite/Melt Partitioning of Samarium, Europium and Gadolinium
This study is part of an ongoing effort to calibrate the pyroxene/melt Eu oxybarometer for conditions relevant to the martian meteorites. There is fairly good agreement between a determinations using equilibria between Fe-Ti oxides and the estimates from Eu anomalies in shergottite augites in tenns of which meteorites are more or less oxidized. The Eu calibration was for angrite composition pyroxenes which are rather extreme. However, application of a calibration for martian composition augites 113 does not significantly reduce the discrepancy between the two methods. One possible reason for this discrepancy is that augites are non-liquidus. The use of pigeonite rather than augite as the oxy-barometer phase is considered. We have conducted experiments on martian composition pigeonite/melt REE partitioning as a function of fO2.
Oxidation State of Nakhlites as inferred from Fe-Ti oxide Equilibria and Augite/Melt Europium Partitioning
Recent studies have shown that Martian magmas had wide range of oxygen fugacities (fO2) and that this variation is correlated with the variation of La/Yb ratio and isotopic characteristics of the Martian basalts, shergottite meteorites. The origin of this correlation must have important information about mantle sources and Martian evolution. In order to understand this correlation, it is necessary to know accurate value of oxidation state of other Martian meteorite groups. Nakhlites, cumulate clinopyroxenites, are another major group of Martian meteorites and have distinctly different trace element and isotopic characteristics from shergottites. Thus, estimates of oxidation state of nakhlites will give us important insight into the mantle source in general. Several workers have estimated oxidation state of nakhlites by using Fe-Ti oxide equilibrium. However, Fe-Ti oxides may not record the oxidation state of the parent melt of the nakhlite because it is a late-stage mineral. Furthermore, there is no comprehensive study which analyzed all nakhlite samples at the same time. Therefore, in this study (1) we reduced the uncertainty of the estimate using the same electron microprobe and the same standards under the same condition for Fe-Ti oxide in 6 nakhlites and (2) we also performed crystallization experiments to measure partition coefficients of Eu into pyroxene in the nakhlite system in order to estimate fO2 when the pyroxene core formed (i.e. Eu oxybarometer [e.g. 2,6]).
Measurements of L-shell X-ray Emission lines of Neonlike Europium on an Electron Beam Ion Trap
We report a measurement of the two X-ray transitions that proceed from the (1s22s22p51∕23d3∕2)J=1 and (1s22s1/22p63p1/2)J =1 upper levels to the (1s22s22p6)J =0 ground level in neonlike Eu53+ (Z = 63), that is, near the previously documented avoided crossing of the two upper levels at Z = 68. The measurement was carried out using the calorimeter spectrometer on the Livermore EBIT-I electron beam ion trap. It affirms the trends set by the neighboring neonlike ions both in terms of the relative intensity of the two lines and in terms of the magnitude of disagreement with theoretical energy level predictions.
Measurement of Transition Probabilities of Europium Using Laser Induced Breakdown Spectroscopy
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Concentrating rare earth elements to phosphate in molten coal ash by a temperature gradient approach
Synthetic coal ash bearing 560 ppm europium oxide, blended with aluminum phosphate, was heat treated above its melting temperature and crystal evolutions with respect to europium concentration under controlled cooling were studied. The sample in a boat crucible was subjected to a temperature gradient of 100 °C across it to cause zone refining effects on crystallization behaviors in the melt (slag). Post analysis found six mineral phases formed from the melt while europium was only present in calcium phosphate, implying the majority of europium was segregated to the calcium phosphate. Europium concentrations in the calcium phosphate phase tended to be higher at zones with higher temperatures: as high as 7200 ppm, a 13-fold increase from the initial concentration.
Analysis of Silver Release from Furnace-Tested TRISO Particles
High temperature testing of intact TRISO particles previously irradiated in the AGR-5/6/7 experiment was performed in the Furnace for Irradiated TRISO Testing (FITT) to directly confirm diffusive release of silver and europium from intact TRISO particles. Testing was conducted from 1,100–1,600°C for exposure times up to 100 h to directly confirm silver through layer release below safety testing temperatures. The FITT analysis showed highest levels of silver release at 1,300–1,400°C which confirms athermal release behaviors previous observed in step-wise and transient safety tests. Additionally, release was non-uniform with some particles releasing a majority of their inventory while others did not appear to release silver under identical testing conditions, which was consistent with historic observations. An assessment of the effective silver diffusion coefficient in the SiC layer was conducted and indicated maximum values in the 1,300–1,400°C range. The magnitude of the calculated diffusion coefficients also exceeded currently accepted diffusion coefficients. The release behavior of europium from intact particles was also analyzed in FITT for at 1,450–1,550°C for 500 h to 750 h. Direct confirmation of europium release below safety testing temperatures was confirmed absent contributions from matrix release. The analysis indicated europium release follows a general Arrhenius behavior and suggests general uniform release and indicates irradiation conditions influence observed release response. Calculated diffusion kinetics agree well with historic experiments.
Research on high Tc superconducting compounds
Mossbauer research using the 21.54 kev resonance radiation of Eu-151 on the high temperature superconductors Bi(2)Ca(0.5)Eu(0.5)Sr(2)CU2O(x), and EuBa(2)CU(3)O(7-x) is performed. For the Bismuth compound the Mossbauer measurements gave a weak signal at room temperature but improved at lower temperatures. Experimental data indicated that europium is located at only one crystallographic site. Isomer shift measurements were .69 + 0.02 mm/s with respect to EuF(3). The linewidth at room temperature was found to be 2.54 mm/s. This value falls within the values observed by other researchers on Eu based 1,2,3 high-Tc compounds. Our results also show the Eu to be trivalent with no trace of divalent europium present. Superconducting europium based 1,2,3 compounds were prepared and measurements completed. Our results show the Eu to be trivalent with no trace of divalent europium present. These compounds had an average isomer shift of .73 mm/s +/- O.02 for all samples made. One of these was irradiated with 3.5 X 10(exp 16) neutrons and a comparison made of the Mossbauer parameters for the irradiated and non-irradiated samples. Experimental results showed no difference between linewidths but a measurable effect was seen for the isomer shift.
Investigating Covalent Bonding in f-elements using Gas-phase Ion Chemistry
Introduction In the reprocessing of f-elements present in used nuclear fuels, a variety of diglycolamides (DGA’s) are used as extractants for actinide partitioning. In particular, the Actinide-Lanthanide Separation (ALSEP) process typically utilizes either the N,N,N’,N’-tetraoctyl diglycolamide (TODGA) or N,N,N',N'-tetra-2-ethylhexyl diglycolamide (T2EHDGA) extractant ligands following the partitioning of uranium and plutonium from used nuclear fuel. To better understand fundamental interactions in these processes, covalent bonding of several f-elements with diglycolamides, primarily TODGA, is investigated in the gas phase using nanospray ionization and a quadrupole time-of-flight mass spectrometer. Further, analysis of the identity and relative strength of the cluster is enabled by MS2 isolation and collision induced dissociation. Methods Metal ion cluster analysis was completed using a Bruker mircOTOF-Q II quadrupole time-of-flight mass spectrometer equipped with a CaptiveSpray nanospray ion source. Metal:ligand solutions were prepared as 30 µM europium nitrate, samarium nitrate, cerium nitrate, or holmium nitrate and 3 µM DGA in acetonitrile or a 50:50 mixture of acetonitrile: isopropanol. Cluster mass spectra and collision-induced dissociation experiments were conducted in positive mode. Preliminary data To examine the patterns and relative strength of lanthanide: DGA interactions, MS2 experiments were completed with each lanthanide species listed above. Preliminary analyses of samarium and europium TODGA clusters suggest several combinations of TODGA and nitrate forming. The samarium cluster experiments yielded Sm(TODGA)x clusters with a samarium:TODGA ratio of up to 1:7 able to be isolated and evidence of greater ratios present in the mass spectrum. This is surprising, as metal clusters are not expected to have a coordination space able to accommodate this many ligands as large as TODGA. MS2 experiments show that, at higher ratios and with sufficient collision energy, entire TODGA ligands are removed instead of being fragmented. These experiments show that a lower collision energy is required to remove ligands as the number of bound TODGA’s increases, suggesting that in larger clusters, ligands are more delicately complexed to the metal. In addition to Sm(TODGA)x, several clusters were observed with nitrate ions bound to the metal in addition to TODGA. With a single nitrate ion, clusters with up to six TODGA’s were able to be isolated. In a similar pattern to the samarium clusters with only TODGA, less collision energy is required to eliminate one or more TODGA’s with increasing size. MS2 experiments suggest clusters with one nitrate appear to be of an equivalent or greater stability to clusters which replace the nitrate with a TODGA, as more collision energy is required to remove a TODGA ligand. These species with one nitrate are also in a higher abundance than the equivalent TODGA only cluster. With two nitrate ions, only clusters with a single TODGA were able to be isolated. Analogous europium experiments resulted in very similar clusters. Ratios of up to 1:7 Eu:TODGA were able to be isolated, and clusters with one nitrate and up to five TODGAs were isolated. In clusters with two nitrate ions, one or two TODGA’s could also be bound to the metal. MS2 experiments suggested, similarly to samarium, that larger clusters required less collision energy to eliminate TODGA. Europium clusters with one nitrate are in greater abundance and are stronger than the equivalent cluster which replaces the nitrate with TODGA. Similar analysis with cerium and holmium is ongoing, as well as analysis with other DGA ligands to compare relative strengths of the lanthanide metals with various extractant ligands.