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At least 37 records · Page 2
All sourcesNASA NTRSDOE OSTI
DOE OSTI2017

Magnetic interactions in praseodymium ruthenate Pr{sub 3}RuO{sub 7} with fluorite-related structure

Solid solutions Pr{sub 3}(Ru{sub 1-x}Ta{sub x})O{sub 7} (0≤x≤1.0) and (Pr{sub 1-x}Y{sub x}){sub 3}RuO{sub 7} (0≤x≤0.7) were obtained as a single phase compound. They crystallize in an orthorhombic superstructure derived from that of the cubic fluorite with space group Cmcm. The results of the Rietveld analysis for X-ray diffraction profiles of Pr{sub 3}(Ru{sub 1-x}Ta{sub x})O{sub 7} showed that Ru and Ta atoms are randomly situated at the six-coordinate 4b site. For (Pr{sub 1-x}Y{sub x}){sub 3}RuO{sub 7}, with increasing the concentration of Y ions (x value), the smaller Y ions occupy selectively the seven-coordinate 8g site rather than the eight-coordinate 4a site. Through magnetic susceptibility measurements for Pr{sub 3}(Ru{sub 1-x}Ta{sub x})O{sub 7}, the antiferromagnetic transition temperatures decrease linearly with increasing x value, and at x=0.75 no magnetic ordering was found down to 1.8 K, indicating the magnetic interaction is not one-dimensional, but three-dimensional. On the other hand, the antiferromagnetic transition temperature for (Pr{sub 1-x}Y{sub x}){sub 3}RuO{sub 7} decreases with increasing x value, but above x≥0.50 it becomes constant (~12 K). This result indicates that Pr{sup 3+} ions at the seven-coordinate site greatly contribute to the antiferromagnetic interactions observed in (Pr{sub 1-x}Y{sub x}){sub 3}RuO{sub 7}. Density functional calculations of Pr{sub 3}RuO{sub 7} demonstrate that the electronic structure gives insulating character and that oxygen 2p orbitals hybridize strongly with Ru 4d orbitals in the valence band (VB). Near the top of VB, the Pr 4 f orbitals at the seven-coordinated site also show a weak hybridization with the O(1) 2p orbitals. The Ru-O(1)-Pr superexchange pathway take part in three-dimensional magnetic interaction and play an important role in an enhancement of long-range magnetic ordering. - Graphical abstract: The spin densities and the spin polarization of Pr{sub 3}RuO{sub 7} are shown. Significant spin polarization is seen on the magnetic Pr and Ru ions, but there is also some on the O(1), (3) ligands of Ru. - Highlights: • New fluorite-related quaternary praseodymium ruthenates were prepared. • Pr{sub 3}RuO{sub 7} shows an antiferromagnetic transition at 55 K. • The Ru-O-Pr superexchange interactions are three-dimensional.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2013

Synthesis and structural studies of praseodymium doped silver borate glasses

Praseodymium doped silver borate glasses with nominal composition xPr{sub 6}O{sub 11}-(25-x)Ag{sub 2}O-75B{sub 2}O{sub 3} (x=0, 1, 2, 3, 4, 5) were prepared by melt quench technique. XRD pattern shows that there is no sharp peak it confirms the amorphous nature of the present glasses. The glass transition temperature (T{sub g}) of this glass system have been studied using the Matac MBS-8000 Digital Signal Processing and Conventional Thermal Analysis (DTA) method. The T{sub g} of these glasses increases with increase in concentration of Pr{sub 6}O{sub 11} except at 0.2 mol%, T{sub g} value is lower. {sup 11}B MAS-NMR shows the presence of sharp peak around 0.306 ppm. Chemical shift of these glasses decreases with mol% of rare earth oxide. FTIR spectra recorded in the region of 400 to 4000 cm{sup -1}. This studies revealed that the progressive addition Ag{sub 2}O and Pr{sub 6}O{sub 11} leads to modification of B{sub 2}O{sub 3} into BO{sub 4} groups. Raman measurements of these glasses support the proposed interpretations of the experimental results.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Electrical properties of praseodymium oxide doped Boro-Tellurite glasses

Glasses of the composition xPr{sub 6}O{sub 11}- (35-x)TeO{sub 2}-65B{sub 2}O{sub 3} (x=0, 0.1 to 0.5 mol %) have been prepared using the melt quenching method. The ac and dc conductivity of glass have been measured over a wide range of frequencies and temperatures. Experimental results indicate that the ac conductivity depend on temperature, frequency and Praseodymium content. The conductivity as a function of frequency exhibited two components: dc conductivity (σ{sub dc}), and ac conductivity (σ{sub ac}). The activation energies are estimated and found to be decreases with composition. The impedance plot at each temperature appeared as a semicircle passes through the origin.

36 MATERIALS SCIENCE↗
DOE OSTI2014

SU-E-T-112: Dose Distribution of Praseodymium-142 Microspheres in Microcapillary Using Radiochromic Film Dosimetry and Applications in Hepatocellular Carcinoma Microsphere Brachytherapy

Purpose: This work verified simulations of beta-minus emitter Praseodymium-142 (Pr-142) for microsphere brachytherapy by performing absolute dose measurements for Pr 142 microspheres in a microcapillary as a simplified model for a single blood vessel for the treatment of Hepatocellular Carcinoma (HCC). Methods: Pr-142 microspheres (mass: 0.169g, average diameter: 29.7±3.9μm) were activated by thermal neutron activation at the University of Missouri Research Reactor. Experimental setup consisted of a microsphere solution (initial activity 36.6mCi in 0.1ml of sterile water) within a glass microcapillary (internal and external diameter: 305μm and 453μm, respectively) placed for 51h in a custom made Gammex Solid Water™ phantom. GAFCHROMIC™ EBT2 film calibrated with a 6MeV electron beam was used to access the dose fall-off of microspheres. The microcapillary was modeled in MCNPX2.6 in order to compare with experiments. Results: The radial dose fall-off on the transverse plane due to scatter and attenuation in the solid water phantom was analyzed using ImageJ for both film and MCNPX2.6 simulations. Isodose analysis showed close agreement among the methods used, i.e. measurements and simulations agree within 3.9% for doses below 1600cGy. Experimental and simulated doses obtained at 0.5 cm radially from the source were 1547cGy and 1610cGy respectively. Discrepancies for points close to the microcapillary surface were observed between MCNPX2.6 and measurements due to film saturation for high doses. Dose due to Pr-142 3.7% gamma emission was below the threshold of detection for the film. Conclusion: A detailed dosimetric study was performed for Pr-142 glass microspheres within a single microcapillary. MCNPX2.6 simulations were verified by means of direct measurement. Based on these results, Pr-142 appears to be a viable choice of radionuclide for treating HCC.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2021

Active Tuning of Optical Constants in the Visible–UV: Praseodymium-Doped Ceria—a Model Mixed Ionic–Electronic Conductor

Mixed ionic-electronic conductors offer chemical and electrical means for active tuning of their optical constants, e.g. with variations in oxygen non-stoichiometry in Pr 0.1 Ce 0.9 O 2-δ , enabling implementation of adaptive thin film optical devices. Here, we demonstrate in-situ chemo-tuning of the extinction coefficient in Pr 0.1 Ce 0.9 O 2-δ at elevated temperatures and provide a tuning model that treats the interdependence of mobile oxygen vacancies and small polarons coupled to variations in optically active praseodymium ions. Further, a new means for electro-tuning of the optical constants of mixed ionic-electronic conductors was demonstrated experimentally and modeled for Pr 0.1 Ce 0.9 O 2-δ thin films deposited on grid-like electrode structures. Modeling of non-steady state optical transmittance modulations in the latter allows for estimation of oxygen vacancy mobility that determines the switching speed of the device. Quenched-in values of nr and k to room temperature become nonvolatile, providing a modulation range in the extinction coefficient of Δk ~0.1 (change of ~800%) and in the refractive index of Δn r ~0.1 (relative to initial n r of ~2.35). Key figures of merit including, transmission optical modulation of ~0.04 per 1 mV nm -1 , switching energy per area of 670 pJ μm -2 and switching times of seconds, were demonstrated, with further improvements possible.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Chemical design of electronic and magnetic energy scales of tetravalent praseodymium materials

Lanthanides in the trivalent oxidation state are typically described using an ionic picture that leads to localized magnetic moments. The hierarchical energy scales associated with trivalent lanthanides produce desirable properties for e.g., molecular magnetism, quantum materials, and quantum transduction. Here, we show that this traditional ionic paradigm breaks down for praseodymium in the tetravalent oxidation state. Synthetic, spectroscopic, and theoretical tools deployed on several solid-state Pr 4+ -oxides uncover the unusual participation of 4f orbitals in bonding and the anomalous hybridization of the 4f 1 configuration with ligand valence electrons, analogous to transition metals. The competition between crystal-field and spin-orbit-coupling interactions fundamentally transforms the spin-orbital magnetism of Pr 4+ , which departs from the J eff = 1/2 limit and resembles that of high-valent actinides. Our results show that Pr 4+ ions are in a class on their own, where the hierarchy of single-ion energy scales can be tailored to explore new correlated phenomena in quantum materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

Elastic anomalies across phase transitions of praseodymium to 12 GPa

The elastic properties of praseodymium (Pr) were investigated at pressures up to 12 GPa at room temperature using ultrasonic interferometry technique. Softening and discontinuities in compressional (P) and shear (S) wave velocities were observed at around 2.5, 6.5 and 10.5 GPa, which are interpreted as indications of the phase transitions from Pr-I (dhcp) to Pr-II (fcc), Pr-II (fcc) to Pr-III (d-fcc) and Pr-III (d-fcc) to Pr-VII (monoclinic or orthorhombic), respectively. Very small discontinuities in compressibility have been observed across the phase transitions of I-II and II-III of Pr, which are unlikely visible in the X-ray diffraction studies. Finally, a comparison with the elastic behaviors of other lanthanide elements (e.g., Ce and La) suggests that the elastic anomalies associated with these phase transitions are likely to be caused by the 6s-5d electron transfer and the softening of acoustic phonon mode facilitated by decreased atomic distances under pressure.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Electrochemistry of Praseodymium in Aqueous Solution Using a Liquid Gallium Cathode

We report the electrochemistry of liquid Ga electrodes in aqueous media was examined in the presence of praseodymium acetate (PrOAc) as an alternate path for low temperature reduction of rare earth elements (REE). This study investigated the aqueous electrochemistry of Ga with and without REEs (Pr). Cyclic voltammetry experiments showed that in the presence of PrOAc, an order of magnitude increase in cathodic current was observed for the Ga electrode, compared to that in the absence of Pr. Decrease in the reduction current with the increase of scan rate, with and without Pr, suggests catalytic reactions following electron transfer, which was attributed to the Ga 2 O disproportionation reaction. Chronoamperometric experiments performed in Pr containing solutions formed a precipitate. Over 50% of the Pr ions from the aqueous electrolyte were immobilized in the precipitate; a solid Ga-rich phase. Formation of this precipitate was only possible when Ga oxidation was induced. This condition was achieved by circulation of liquid Ga from the pool via external pump and returned dropwise to the liquid Ga pool. When the collected precipitate was leached in dilute HCl, Pr was released with H 2 evolved as a byproduct, and Ga returned to its initial liquid metallic state. These preliminary results show encouraging new routes that could be applied for the recovery of diluted REE leachates, such as those obtained from magnets, coal fly ash, and ores.

25 ENERGY STORAGE↗
NASA NTRS1995

High Temperature Superconductivity in Praseodymium Doped (0%, 2%, 4%) in Melt-Textured Y(1-x)Pr(x)Ba2Cu3O(7-delta) Systems

A study of the magnetic and structural properties of the alloy Y(1-x)Pr(x)Ba2Cu3O(7-delta) of 0%, 2%, and 4% doping of praseodymium is presented. The resulting oxides of the alloy series are a high-temperature superconductor Y-Ba-Cu-O, which has an orthorhombic superconducting crystal-lattice. Magnetic relaxation studies have been performed on the Y-Pr-Ba-CuO bulk samples for field orientation parallel to the c-axis, using a vibrating sample magnetometer. Relaxation was measured at several temperatures to obtain the irreversible magnetization curves used for the Bean model. Magnetization current densities were derived from the relaxation data. Field and temperature dependence of the logarithmic flux-creep relaxation was measured in critical state. The data indicates that the effective activation energy U(eff) increases with increasing T between 77 K and 86 K. Also, the data shows that U(eff)(T) and superconducting transition temperature, Tc, decreased as the lattice parameters increased with increasing Pr ion concentration, x, for the corresponding Y(1-x)Pr(x)Ba(x)Cu3O(7-delta) oxides. One contribution to Tc decrease in this sampling is suspected to be due to the larger ionic radius of the Pr(3+) ion. The upper critical field (H(sub c2)) was measured in the presence of magnetic field parallel to the c axis. A linear temperature dependence with H(sub c2) was obtained.

James, Claudell↗
DOE OSTI2014

Elastic properties of silver borate glasses doped with praseodymium oxide

A series of glasses xPr{sub 6}O{sub 11−}(35−x) Ag{sub 2}O−65B{sub 2}O{sub 3} with x=0, 0.1, 0.2, 0.3, 0.4 and 0.5 mol % were synthesized by melt quenching technique. Longitudinal and shear ultrasonic velocity were measured at 5 MHz frequency and at room temperature. Elastic moduli, Poisson's ratio and Debye temperature have been calculated from the measured density and ultrasonic velocity at room temperature. The experimental results indicate that the elastic constants depend upon the composition of the glasses. The role of the Pr{sub 6}O{sub 11} inside the glass network was discussed.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2019

Effect of Praseodymium and Lanthanum Substitution for Bismuth on the Thermoelectric Properties of BiCuSeO Oxyselenides

The results of investigating the thermoelectric properties of the bulk р-type oxyselenides Bi{sub 1 –x}Pr{sub x}CuSeO (x = 0, 0.04, 0.08) and Bi{sub 0.96}La{sub 0.04}CuSeO obtained by the solid-state reaction technique are presented. The temperature dependences of the thermopower, electrical resistivity, and thermal conductivity are measured at temperatures from room temperature to 800 K. Over the whole temperature range, a decrease in the electrical resistivity and thermopower is observed with increasing substitution level, while the thermal conductivity is almost unaffected by the substitution of rare-earth elements for bismuth. Despite the nominal valence of Bi, La, and Pr being the same, the replacement of bismuth by rare-earth ions leads to an increase in the charge-carrier concentration, which may be caused by a difference in the electronic configurations of ions, resulting in a shift of the Fermi level to the valence band.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Temporal and spatial tuning of optical constants in praseodymium doped ceria by electrochemical means

Abstract Temporal and spatial tuning of the refractive index of optical thin films is desired for flat optics applications. The redistribution of mobile ions in mixed ionic-electronic conductors (MIEC) has been demonstrated to serve as a viable means for achieving optical tuning down to the nanoscale. Here we studied the dynamic range of the optical tuning achievable in the refractive index, in the MIEC oxide – Pr x Ce 1− x O 2− δ (PCO), for x = 0.1, 0.2 and 0.4, at 500 °C, by in-situ spectrophotometry. Significant increases in the modulation of both the imaginary and real optical constants in the visible and the adjacent spectra were obtained for increased doping levels. Device employing an electrochemical titration method was implemented to modulate the oxygen concentration, and thereby the optical transmission of PCO. Incorporation of a patterned top electrode allowed for the demonstration of spatial control of PCO thin film properties by in-situ video imaging of the optical switching process. The electrochemically induced optical state is shown to remain non-volatile upon quenching the device to room temperature under applied bias.

36 MATERIALS SCIENCE↗