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At least 37 records · Page 2
All sourcesNASA NTRSDOE OSTI
NASA NTRS2012

Metasomatic Control of Water in Garnet and Pyroxene from Kaapvaal Craton Mantle Xenoliths

Fourier transform infrared spectrometry (FTIR) and laser ablation inductively coupled plasma mass spectrometry (LA-ICPMS) were used to determine water, rare earth (REE), lithophile (LILE), and high field strength (HFSE) element contents in garnet and pyroxene from mantle xenoliths, Kaapvaal craton, southern Africa. Water enters these nominally anhydrous minerals as protons bonded to structural oxygen in lattice defects. Pyroxene water contents (150-400 ppm in clinopyroxene; 40-250 ppm in orthopyroxene) correlate with their Al, Fe, Ca and Na and are homogeneous within a mineral grains and a xenolith. Garnets from Jagersfontein are chemically zoned for Cr, Ca, Ti and water contents. Garnets contain 0 to 20 ppm H2 Despite the fast diffusion rate of H in mantle m inerals, the observations above indicate that the water contents of mantle xenolith minerals were not disturbed during kimberlite entrainment and that the measured water data represent mantle values. Trace elements in all minerals show various degrees of light REE and LILE enrichments indicative of minimal to strong metasomatism. Water contents of peridotite minerals from the Kaapvaal lithosphere are not related to the degree of depletion of the peridotites. Instead, metasomatism exerts a clear control on the amount of water of mantle minerals. Xenoliths from each location record specific types of metasomatism with different outcomes for the water contents of mantle minerals. At pressures . 5.5 GPa, highly alkaline melts metasomatized Liqhobong and Kimberley peridotites, and increased the water contents of their olivine, pyroxenes and garnet. At higher pressures, the circulation of ultramafic melts reacting with peridotite resulted in co-variation of Ca, Ti and water at the edge of garnets at Jagersfontein, overall decreasing their water content, and lowered the water content of olivines at Finsch Mine. The calculated water content of these melts varies depending on whether the water content of the peridotite (2 wt% HO. 2O) or individual m inerals (<0.5-13 wt% H2O) are used, and also depend on the mineral-melt water partition coefficients. These metasomatic events are thought to have occurred during the Archean and Proterozoic, meaning that the water contents measured here have been preserved since that time and can be used to investigate viscocity and longevity of cratonic mantle roots.

Peslier, Anne H.↗
DOE OSTI2021

Ultrafast measurements of the interfacial spin Seebeck effect in Au and rare-earth iron-garnet bilayers

We investigate picosecond spin-currents across Au/iron-garnet interfaces in response to ultrafast laser heating of the electrons in the Au film. In the picoseconds after optical heating, interfacial spin currents occur due to an interfacial temperature difference between electrons in the metal and magnons in the insulator. We report measurements of this interfacial longitudinal spin Seebeck effect between Au and rare-earth iron-garnet insulators, i.e. RE 3 Fe 5 O 12 , where RE is Y, Eu, Tb, Tm. By systematically varying the rare-earth element, we modify the total magnetic moment of the iron-garnet. We use time domain thermoreflectance (TDTR) measurements to characterize the thermal response of the bilayer to ultrafast optical heating. We use time-resolved magneto-optic Kerr effect (TR-MOKE) measurements of the Au layer to measure the time-evolution of spin accumulation in the Au film. Replacing Y with other rare-earths enhances the electron-magnon conductance G e-m at the Au iron-garnet interface by as much as a factor of three. The electron-magnon conductance does not follow the trend of either the total magnetization of the iron garnet or the magnetic moment of the rare-earth.

36 MATERIALS SCIENCE↗
DOE OSTI2021

3D Printed, Low Tortuosity Garnet Framework For Beyond 500 Wh/kg Batteries

In this project, we developed LLZO garnet ink recipes and processes for 3D-printing highly ordered ionically conductive garnet porous structures on dense garnet separators. Using this technique, we are able to fabricate controlled architecture LLZO garnet solid-state electrolyte (SSE) trilayers for application in solid-state lithium batteries. The trilayer comprises a thin dense center layer sandwiched between a 3D-printed patterned porous layer and a random porous layer. The dense layer functions as the ionic separator between the anode and cathode. The random porous layer hosts the lithium-metal anode and provides the structural support. The 3D-printed SSE patterned porous layer hosts the cathode, providing continuous, low tortuosity pathways for fast 3D Li+ transport through the cell while increasing the electrode/electrolyte interface area to decrease the interfacial resistance. Compared to the random porous structure, this ordered patterned structure possesses more vacant space for higher cathode loading without sacrificing ionically conducting capability, thus potentially greatly increasing the cell energy density. For demonstration purposes, we developed two patterns for the 3D-printed porous layer: grids and columns, for hosting sulfur and NMC cathode, respectively. The corresponding two types of cells were fabricated and tested, and have demonstrated achievement of theoretical discharge capacity without cathode calendaring. In addition, we developed a fundamental solid-state ionic and electronic transport model to optimize the 3D-printed structures for maximum energy and power density. The model was validated by experiment and provides the critical design criteria for achieving the >500 Wh/kg energy goal as function of C-rate.

25 ENERGY STORAGE↗
NASA NTRS1981

Partition coefficients for REE between garnets and liquids - Implications of non-Henry's Law behaviour for models of basalt origin and evolution

An experimental investigation of Ce, Sm and Tm rare earth element (REE) partition coefficients between coexisting garnets (both natural and synthetic) and hydrous liquids shows that Henry's Law may not be obeyed over a range of REE concentrations of geological relevance. Systematic differences between the three REE and the two garnet compositions may be explained in terms of the differences between REE ionic radii and those of the dodecahedral site into which they substitute, substantiating the Harrison and Wood (1980) model of altervalent substitution. Model calculations demonstrate that significant variation can occur in the rare earth contents of melts produced from a garnet lherzolite, if Henry's Law partition coefficients do not apply for the garnet phase.

Harrison, W. J.↗
NASA NTRS1982

Experimental determination of the spinel-garnet boundary in a Martian mantle composition

The high pressure reaction orthopyroxene + clinopyroxene + spinel to garnet + olivine is applicable to the mantle of Mars. Experimental reversals of this reaction in the system CaO-MgO-FeO-Al2O3-SiO2 have been made in the range 1000-1200 C using the bulk composition proposed by Morgan and Anders (1980). At 1000 C, 1100 C, and 1200 C the garnet-out equilibrium is bracketed at 10.8 + or - 0.5, 12.6 + or - 0.5, and 15.2 + or - 0.5 kbars, respectively. A dP/dT slope of 14.0 bar/K at 1000 C increasing to 26.0 bar/K at 1200 C has been inferred. Depending on bulk composition, the mantle of Mars is inferred to have a phase assemblage of either olivine + clinopyroxene + orthopyroxene + garnet or olivine + clinopyroxene + garnet + spinel. In the second, the partial melts will not be buffered by olivine and orthopyroxene and will have markedly lower silica activities than those of the terrestrial mantle.

Patera, E. S.↗
NASA NTRS1994

Computational modelling of Er(3+): Garnet laser materials

The Er(3+) ion has attracted a lot of interest for four reasons: (1) Its (4)I(sub 13/2) yields (4)I(sub 15/2) transition lases in the eyesafe region near 1.5 micron; (2) the (4)I(sub 13/2) transition lases near 2.8 micron, an important wavelength for surgical purposes; (3) it displays surprisingly efficient upconversion with lasing observed at 1.7, 1.2, 0.85, 0.56, 0.55, and 0.47 micron following 1.5 micron pumping; and (4) it has absorption bands at 0.96 and 0.81 micron and thus can be diode pumped. However, properties desirable for upconversion reduce the efficiency of 1.5 and 3 micron laser operation and vice versa. Since all of the processes are influenced by the host via the crystal field induced stark splittings in the Er levels, this project undertook modelling of the host influence on the Er lasinng behavior. While growth and measurement of all ten Er(3+) doped garnets is the surest way of identifying hosts which maximize upconversion (or conversly, 1.5 and 3 micron performance), it is also expensive - costing approximately $10,000/material or approximately $100,000 for the materials computationally investigated here. The calculations were performed using a quantum mechanical point charge model developed by Clyde Morrison at Harry Diamond Laboratories. The programs were used to fit the Er:YAG experimental energy levels so that the crystal field parameters, B(sub nm) could be extracted. From these radial factors, rho (sub n) were determined for Er(3+) in garnets. These, in combination with crystal field components, Anm, available from X-ray data, were used to predict energy levels for Er in the other nine garnet hosts. The levels in Er:YAG were fit with an rms error of 12.2/cm over a 22,000/cm range. Predicted levels for two other garnets for which literature values were available had rms errors of less than 17/cm , showing the calculations to be reliable. Based on resonances between pairs of calculated stark levels, the model predicts GSGG as the best host for 1.5 micron laser operation, GSGG or YSAG as the best host for a 2.8 micron operation, and LuGG as the best host for an upconversion material.

Spangler, Lee H.↗
NASA NTRS1994

MgSiO3-FeSiO3-Al2O3 in the Earth's lower mantle: Perovskite and garnet at 1200 km depth

Natural pyroxene and garnet starting material are used to study the effects of joint Fe and Al substitution into MgSiO3 perovskite at approxmiately 50 GPa. Garnet is found to coexist with perovskite in samples containing both Fe and Al to pressures occurring deep into the lower mantel (approximately 1200 km depth). The volume of the perovskite unit cell is V(sub o(Angstrom(exp 3)) = 162.59 + 5.95x(sub FeSiO3) + 10.80x(sub Al2O3) with aluminum causing a significant increase in the distortion from the ideal cubic cell. On the basis of a proposed extension of the MgSiO3-Al2O3 high-pressure phase diagram toward FeSiO3, Fe is shown to partition preferentially into the garnet phase. The stability of garnet deep into the lower mantel may hinder the penetration of subducted slabs below the transition zone.

O'Neill, Bridget↗
NASA NTRS1994

Rare Earth Garnet Selective Emitter

Thin film Ho-YAG and Er-YAG emitters with a platinum substrate exhibit high spectral emittance in the emission band (epsilon(sub lambda) approx. = 0.75, sup 4)|(sub 15/2) - (sup 4)|(sub 13/2),for Er-YAG and epsilon(sub lambda) approx. = 0.65, (sup 5)|(sub 7) - (sup 5)|(sub 8) for Ho-YAG) at 1500 K. In addition, low out-of-band spectral emittance, epsilon(sub lambda) less than 0.2, suggest these materials would be excellent candidates for high efficiency selective emitters in thermophotovoltaic (TPV) systems operating at moderate temperatures (1200-1500 K). Spectral emittance measurements of the thin films were made (1.2 less than lambda less than 3.0 microns) and compared to the theoretical emittances calculated using measured values of the spectral extinction coefficient. In this paper we present the results for a new class of rare earth ion selective emitters. These emitters are thin sections (less than 1 mm) of yttrium aluminum garnet (YAG) single crystal with a rare earth substitutional impurity. Selective emitters in the near IR are of special interest for thermophotovoltaic (TPV) energy conversion. The most promising solid selective emitters for use in a TPV system are rare earth oxides. Early spectral emittance work on rare earth oxides showed strong emission bands in the infrared (0.9 - 3 microns). However, the emittance outside the emission band was also significant and the efficiency of these emitters was low. Recent improvements in efficiency have been made with emitters fabricated from fine (5 - 10 microns) rare earth oxide fibers similar to the Welsbach mantle used in gas lanterns. However, the rare earth garnet emitters are more rugged than the mantle type emitters. A thin film selective emitter on a low emissivity substrate such as gold, platinum etc., is rugged and easily adapted to a wide variety of thermal sources. The garnet structure and its many subgroups have been successfully used as hosts for rare earth ions, introduced as substitutional impurities, in the development of solid state laser crystals. Doping, dependent on the particular ion and crystal structure, may be as high as 100 at. % (complete substitution of yttrium ion with the rare earth ion). These materials have high melting points, 1940 C for YAG (Yttrium Aluminum Garnet), and low emissivity in the near infrared making them excellent candidates for a thin film selective emitter. As previously stated, the spectral emittance of a rare earth emitter is characterized by one or more well defined emission bands. Outside the emission band the emittance(absorptance) is much lower. Therefore, it is expected that emission outside the band for a thin film selective emitter will be dominated by the emitter substrate. For an efficient emitter (power in the emission band/total emitted power) the substrate must have low emittance, epsilon(sub S). This paper presents normal spectral emittance, epsilon(sub lambda), measurements of holmium(Ho) and erbium (Er) doped YAG thin film selective emitters at (1500 K), and compares those results with the theoretical spectral emittance.

Lowe, Roland A.↗
DOE OSTI2022

Rapid pyrolysis to form super ionic conducting lithium garnets

A method of preparing a lithium-ion conducting garnet via low-temperature solid-state synthesis is disclosed. The lithium-ion conducting garnet comprises a substantially phase pure aluminum-doped cubic lithium lanthanum zirconate (Li 7 La 3 Zr 2 O 14 ). The method includes preparing nanoparticles comprising lanthanum zirconate (La 2 Zr 2 O 7 -np) via pyrolysis-mediated reaction of lanthanum nitrate (La(NO 3 ) 3 ) and zirconium nitrate (Zr(NO 3 ) 4 ). The method also includes pyrolyzing a solid-state mixture comprising the La 2 Zr 2 O 7 -np, lithium nitrate (LiNO 3 ), and aluminum nitrate (Al(NO 3 ) 3 ) to give the Li 7 La 3 Zr 2 O 14 and thereby prepare the lithium-ion conducting garnet. A lithium-ion conducting garnet prepared via the method is also disclosed.

Daemen, Luc L.↗
DOE OSTI2023

Codoping method for modifying the scintillation and optical properties of garnet-type scintillators

A method of tailoring the properties of garnet-type scintillators to meet the particular needs of different applications is described. More particularly, codoping scintillators, such as Gd 3 Ga 3 Al 2 O 12 , Gd 3 Ga 2 Al 3 O 12 , or other rare earth gallium aluminum garnets, with different ions can modify the scintillation light yield, decay time, rise time, energy resolution, proportionality, and/or sensitivity to light exposure. Also provided are the codoped garnet-type scintillators themselves, radiation detectors and related devices comprising the codoped garnet-type scintillators, and methods of using the radiation detectors to detect gamma rays, X-rays, cosmic rays, and particles having an energy of 1 keV or greater.

Tyagi, Mohit↗
DOE OSTI2023

Revealing Site Occupancy in a Complex Oxide: Terbium Iron Garnet

Complex oxide films stabilized by epitaxial growth can exhibit large populations of point defects which have important effects on their properties. The site occupancy of pulsed laser-deposited epitaxial terbium iron garnet (TbIG) films with excess terbium (Tb) is analyzed, in which the terbium:iron (Tb:Fe)ratio is 0.86 compared to the stoichiometric value of 0.6. The magnetic properties of the TbIG are sensitive to site occupancy, exhibiting a higher compensation temperature (by 90 K) and a lower Curie temperature (by 40 K) than the bulk Tb 3 Fe 5 O 12 garnet. Data derived from X-ray core-level spectroscopy, magnetometry, and molecular field coefficient modeling are consistent with occupancy of the dodecahedral sites by Tb 3+ , the octahedral sites by Fe 3+ , Tb 3+ and vacancies, and the tetrahedral sites by Fe 3+ and vacancies. Energy dispersive X-ray spectroscopy in a scanning transmission electron microscope provides direct evidence of Tb Fe antisites. A small fraction of Fe 2+ is present, and oxygen vacancies are inferred to be present to maintain charge neutrality. In conclusion, variation of the site occupancies provides a path to considerable manipulation of the magnetic properties of epitaxial iron garnet films and other complex oxides, which readily accommodate stoichiometries not found in their bulk counterparts.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Thermally generated magnonic spin currents in a polycrystalline gadolinium iron garnet thin film with perpendicular magnetic anisotropy

Rare-earth iron garnets (REIGs) are the benchmark systems for magnonics, including the longitudinal spin Seebeck effect (LSSE). While most research has focused on single-crystalline REIGs on complimentary garnet substrates, moving to more, cost-effective complementary metal-oxide semiconductor (CMOS)-compatible substrates is important to integrate REIG thin films with existing technology. In this regard, we grow a 130 nm-thick polycrystalline gadolinium iron garnet (GdIG) film on the Si/SiO2 substrate and investigate the temperature-dependent LSSE. Interestingly, the polycrystalline GdIG film exhibits perpendicular magnetic anisotropy (PMA) at room temperature which is induced by tensile in-plane (IP)-strain originating from the thermal-expansion mismatch between the GdIG film and the substrate during rapid thermal annealing. Further, a spin-reorientation transition from the out-of-plane IP direction below TS = 180 K is observed. Additionally, the film reveals a magnetic compensation temperature, TComp, of ≈240 K. The LSSE voltage not only demonstrates a sign-inversion around TComp, but also shows noticeable changes around TS. As compared to a single-crystalline GdIG film, the lower LSSE voltage for the polycrystalline GdIG is attributed to the higher effective magnetic anisotropy and enhanced magnon scattering at the grain boundaries. Our study not only paves the way for the cost-effective growth of CMOS-compatible REIG-based systems with PMA for magnonic memory and information processing applications, but also highlights the fact that the spincaloritronic and spin-insulatronic properties of the polycrystalline REIGs follow those of their single-crystalline counterparts with reduced spin-to-charge conversion efficiency through LSSE which can be tuned further by controlling the average gran size and interface engineering.

Physics↗
DOE OSTI2024

Interfacial magnetic characteristics of nearly compensated gadolinium iron garnet

Reports on spin Hall magnetoresistance, magnonic spin currents from thermal gradients, and spin transfertorque magnetic random-access memory using compensated ferrimagnets largely discuss bulk magnetization but lack consideration of depth profiles or interfacial characteristics. Here, magnetic and structural characterization of profiles and interfaces was performed for nearly compensated gadolinium iron garnet (GdIG) thin films. X-ray diffraction and reciprocal space maps show that sputter deposited GdIG on Si is polycrystalline with the desired cubic garnet phase, and GdIG on gadolinium gallium garnet (GGG) is epitaxial with <0.06% compressive strain. Temperature-dependent magnetometry confirms the compensation temperatures of GGG/GdIG and Si/GdIG to be 285 and 260 K, respectively, both near room temperature. Interestingly, these measurements suggest the presence of unsaturated rare-earth moments, which result in a characteristic hysteresis between heating and cooling sequences in the magnetization-temperature curves at zero field. Depth-profile measurements from polarized neutron reflectometry (PNR) indicate up to 91% volume fraction in GdIG on Si. At the interface, PNR reveals a region containing magnetized Fe-doped GGG, a low-density GdIG at the GGG/GdIG interface, and a thin magnetically dead layer at the Si/GdIG interface. Cross-sectional transmission electron microscopy and energy dispersive x-ray spectroscopy confirm the assessment of PNR. In conclusion, the magnetic characteristics of interfacial regions are attributed to intermixing of Fe-Ga at the GGG/GdIG interface and the presence of amorphous Fe-Si at the Si/GdIG interface.

36 MATERIALS SCIENCE↗
NASA NTRS1974

Characteristics of epitaxial garnets grown by CVD using single metal alloy sources

Single metal alloys have been explored as the cation source in the chemical vapor deposition (CVD) of iron garnets. Growth of good quality single crystal garnet films containing as many as five different cations has been achieved over a wide range of deposition conditions. The relationship of film composition to alloy compositions and deposition conditions has been determined for several materials. By proper choice of the alloy composition and the deposition conditions, uncrazed deposits were grown on (111) gadolinium gallium garnet (GGG) substrates. Data on physical, magnetic and optical properties of representative films is presented and discussed.

Besser, P. J.↗
NASA NTRS1983

Solidus and liquidus temperatures and mineralogies for anhydrous garnet-lherzolite to 15 GPa

Strong convergence is noted, in experimental data for systems pertaining to anhydrous fertile garnet-lherzolite in the 6.5-15 GPa range, either to a common temperature or to temperatures differing by only about 100 C. The major element composition of magmas generated by even minor degrees of partial melting may be similar to the composition of the primordial, bulk silicate earth in an upper mantle stratigraphic column more than 160 km deep. Whether or not the solidus and liquidus intersect, the liquidus mineralogy for undepleted garnet-lherzolite compositions is found to change from olivine, at low pressures, to pyroxene, garnet, or a solid solution of both, at pressures greater than 10-15 GPa.

Herzberg, C. T.↗
NASA NTRS1988

Martian mantle primary melts - An experimental study of iron-rich garnet lherzolite minimum melt composition

The minimum melt composition in equilibrium with an iron-rich garnet lherzolite assemblage is ascertained from a study of the liquidus relations of iron-rich basaltic compositions at 23 kb. The experimentally determined primary melt composition and its calculated sodium content reveal that Martian garnet lherzolite minimum melts are picritic alkali olivine basalts. Martian primary melts are found to be more picritic than terrestrial garnet lherzolite primary melts.

Bertka, Constance M.↗
NASA NTRS1999

Rare Earth Doped Yttrium Aluminum Garnet (YAG) Selective Emitters

As a result of their electron structure, rare earth ions in crystals at high temperature emit radiation in several narrow bands rather than in a continuous blackbody manner. This study presents a spectral emittance model for films and cylinders of rare earth doped yttrium aluminum garnets. Good agreement between experimental and theoretical film spectral emittances was found for erbium and holmium aluminum garnets. Spectral emittances of films are sensitive to temperature differences across the film. For operating conditions of interest, the film emitter experiences a linear temperature variation whereas the cylinder emitter has a more advantageous uniform temperature. Emitter efficiency is also a sensitive function of temperature. For holminum aluminum garnet film the efficiency is 0.35 at 1446K but only 0.27 at 1270 K.

Chubb, Donald L.↗
DOE OSTI2025

Czochralski Growth and Characterization of a Compositionally Complex Rare Earth Aluminum Garnet Scintillator: (Gd 1/4 Y 1/4 Tb 1/4 Lu 1/4 ) 3 Al 5 O 12 :Ce

Compositionally complex oxides have garnered increasing interest for their enhanced phase stability and tunable functional properties, yet their development as bulk single crystal scintillators remains limited. Herein, we report the Czochralski growth and characterization of (Gd 1/4 Y 1/4 Tb 1/4 Lu 1/4 ) 3 Al 5 O 12 :Ce (GYTLAG), a compositionally complex garnet incorporating four dodecahedrally coordinated principal rare earth elements. The garnet phase was confirmed by powder and single crystal X-ray diffraction, and macroscopic defects are described. X-ray absorption near-edge structure measurements confirm the 3+ oxidation state of all rare earths and support their occupation of the same crystallographic site; white line intensity variations correlate with the anticipated segregation behavior. Elemental segregation is quantified by SEM/EDS and ICP-OES, and a linear trend was established between the segregation coefficient and the difference between each rare earth’s ionic radius (r) and the average ionic radius (AIR) of the dodecahedral site. This trend offers a predictive framework for compositional control in future REAG crystals grown by the Czochralski method. Photoluminescence and radioluminescence measurements reveal both Ce 3+ and Tb 3+ emission. Scintillation pulses exhibit four-component decay with dominant ~230 µs and ~1.2 ms components, and the light yield is estimated to be up to 43,000 ph/MeV under 137Cs γ-ray excitation. GYTLAG also demonstrates a strong radioluminescence efficiency and 50% lower afterglow at 20 ms compared to a LuAG:Ce reference, underscoring its promise for scintillator applications.

Compositionally complex oxide, high entropy oxide,↗