Experimental and computational phase boundary mapping of Co 4 Sn 6 Te 6
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Caitlin M. Crawford↗
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Co(x)Ni(4-x)Sb(12-y)Sn(y) Ternary Skutterudites: Processing and Thermoelectric Properties
Skutterudites have proven to be a useful thermoelectric system as a result of their high figure of merit, favorable mechanical properties, and good thermal stability. Binary skutterudites have received the majority of interest in recent years, as a result of successful double and triple filling schemes. Ternary skutterudites, such as Ni4Sb7Sn5, also demonstrate good thermoelectric performance, with high power factor and low thermal conductivity. Ternary skutterudites, as contrasted to binary systems, provide more possibility for tuning electronic structure as substitutions can be studied on three elements. The Co(x)Ni(4-x)Sb(12-y)Sn(y) system has been investigated as both a p- and n-type thermoelectric material, stable up to 200 C. The system is processed through a combination of solidification, mechanical alloying, and hot pressing steps. Rietveld structure refinement has revealed an interesting occupancy of Sn on both the 24g Wyckoff position with Sb as well as the 2a position as a rattler. In addition to thermoelectric properties, detailed processing routes have been investigated on the system.
Seebeck effect↗
Thermoelectric properties of Co(x)Ni(4-x)Sb(12-y)Sn(y) ternary skutterudites
Thermoelectric materials based on the skutterudite crystal structure have demonstrated enhanced performance (ZT greater than 1), along with good thermal stability and favorable mechanical properties. Binary skutterudites, with single and multiple fillers, have been intensively studied in recent years. Compared to binary skutterudites, the ternary systems have received less attention, e.g. Ni4Sb8Sn4. Ternary skutterudites are isoelectronic variants of binary skutterudites; cation substitutions appear to be isostructural to their binary analogues. In general, ternary skutterudites exhibit lower thermal conductivity. Ternary systems of Ni4Bi8Ge4, Ni4Sb8Ge4, and Ni4Sb8Sn4 were investigated using combined solidification and sintering steps. Skutterudite formation was not achieved in the Ni4Bi8Ge4 and Ni4Sb8Ge4 systems; skutterudite formation occurred in Ni4Sb8Sn4 system. P-type material was achieved by Co substitution for Ni. Thermoelectric properties were measured from 298 K to 673 K for Ni4Sb8Sn4, Ni4 Sb7Sn5 and Co2Ni2Sb7Sn5. N-type Ni4Sb8Sn4 exhibit the highest figure of merit of 0.1 at 523 K.
Seebeck Effect↗
Filled Co (sub X) Ni (sub 4-x) Sb (sub 12-y) Sn (sub Y) Skutterudites: Processing and Thermoelectric Properties
Skutterudites have proven to be a useful thermoelectric system as a result of their enhanced figure of merit (ZT1), cheap material cost, favorable mechanical properties, and good thermal stability. The majority of skutterudite interest in recent years has been focused on binary skutterudites like CoSb3 or CoAs3. Binary skutterudites are often double and triple filled, with a range of elements from the lanthanide series, in order to reduce the lattice component of thermal conductivity. Ternary and quaternary skutterudites, such as Co4Ge6Se6 or Ni4Sb8Sn4, provide additional paths to tune the electronic structure. The thermal conductivity can further be improved in these complex skutterudites by the introduction of fillers. The Co (sub X) Ni (sub 4-x) Sb (sub 12-y) Sn (sub Y) system has been investigated as both a p- and n-type thermoelectric material, and is stable up to 200 degrees Centigrade. Yb, Ce, and Dy fillers have been introduced into the skutterudite to study the influence of both the type and the quantity of fillers on processing conditions and thermoelectric properties. The system was processed through a multi-step technique that includes solidification, mechano-chemical alloying, and hot pressing which will be discussed along with thermoelectric transport properties.
Thermoelectricity↗
High-resolution mid-infrared spectra of Co II, Ni I, and Fe II in SN 1987A
Ground-based infrared observations of SN 1987A on day 612 after the explosion have yielded resolved line profiles of Co II, Ni I, Fe II at 10.52, 11.31, and 17.94 micron, respectively. The spectra were taken at a resolving power of about 1000 with an array grating spectrometer on the 4 m telescope of Cerro Tololo Inter-American Observatory. Based on the observed line intensities we have estimated the minimum mass of each ion: M(Co II) = (6.0 +/- 1.8) x 10 exp -5 solar mass; M(Ni I) = (1.1 +/- 0.1) x 10 exp -3 solar mass; and M(Fe II) = (8.0 +/- 1.5) x 10 exp -3 solar mass. From these we infer total masses for cobalt, nickel, and iron in the ejecta. The nickel and iron line profiles are markedly asymmetric. We interpret these as arising from two components, one centered on the stellar rest velocity with an approximately 3250 km/s full width, and the second at about +1200 km/s with an approximately 1100 km/s full width. The asymmetry may represent a large-scale fracturing of the ejecta by Rayleigh-Taylor instabilities.
Jennings, D. E.↗
ASASSN-15LH: A Superluminous Ultraviolet Rebrightening Observed by Swift and Hubble
We present and discuss ultraviolet and optical photometry from the Ultraviolet/Optical Telescope, X-ray limits from the X-Ray Telescope on Swift, and imaging polarimetry and ultraviolet/optical spectroscopy with the Hubble Space Telescope, all from observations of ASASSN-15lh. It has been classified as a hydrogen-poor superluminous supernova (SLSN I), making it more luminous than any other supernova observed. ASASSN-15lh is not detected in the X-rays in individual or co-added observations. From the polarimetry we determine that the explosion was only mildly asymmetric. We find the flux of ASASSN-15lh to increase strongly into the ultraviolet, with an ultraviolet luminosity 100 times greater than the hydrogen-rich, ultraviolet-bright SLSN II SN2008es. We find that objects as bright as ASASSN-15lh are easily detectable beyond redshifts of ∼4 with the single-visit depths planned for the Large Synoptic Survey Telescope. Deep near-infrared surveys could detect such objects past a redshift of ∼20, enabling a probe of the earliest star formation. A late rebrightening-most prominent at shorter wavelengths -is seen about two months after the peak brightness, which is itself as bright as an SLSN. The ultraviolet spectra during the rebrightening are dominated by the continuum without the broad absorption or emission lines seen in SLSNe or tidal disruption events (TDEs) and the early optical spectra of ASASSN-15lh. Our spectra show no strong hydrogen emission, showing only Lyα absorption near the redshift previously found by optical absorption lines of the presumed host. The properties of ASASSN-15lh are extreme when compared to either SLSNe or TDEs.
Brown, Peter J.↗
Multi-Anvil Experimentation Applied to Planetary Differentiation
Planets undergo differentiation that includes segregation of metal from silicate at high temperatures and pressures ranging from deep planetary core pressures (>300 GPa for Earth)to very shallow conditions of asteroids (<100 MPa).The multi-anvil solid media apparatus accesses the middle part of this range from 3 to 30 GPa –pressure relevant to the interior of Mercury, Venus, Earth, Earth’s Moon, and Mars. Early planets are thought to have experienced high temperatures from a combination of heat sources including radioactive decay, gravitational and accretional heating, and impact processes. These heating events led to melting of mantles and cores, thus requiring an understanding of solid-liquid equilibria in metal-silicate systems. In 2006 we established a multi-anvil facility at NASA-JSC combining an 880 ton press and a Kawai/Walker type module from Rockland Research. Our high PT work has been greatly facilitated by use of the COMPRES multi-anvil assemblies (1). Our recent work has included studies of element partitioning between liquid metal and liquid silicate(e.g., 2), as well as between minerals and melts(e.g., 3), both of which have led to better constraints on the timing and conditions of planetary differentiation(e.g. 4). Several examples involving sustained efforts will be summarized below and for the presentation. The distribution of siderophile (iron-loving) elements between core and mantle is controlled by metal-silicate equilibrium across a wide range of pressures. Therefore, experimentation across this pressure range helps to calibrate elemental partitioning models that can be applied to planets, and used to predict mantle chemistry and composition during planetary differentiation. Our studies have focused on a wide range of siderophile elements (refractory Ni, Co, W, Mo; volatile P, Ga, Cu, Sn, Sb; highly siderophile Au, Pd) that have constrained partitioning, valence, and isotopic fractionation, and applied to Earth, Moon, and Mars. When molten mantles (magma oceans) cool enough to initiate crystallization, the solids precipitate at depth and in large planets this involves high pressure phases like garnet, majorite, akimotoite, and ringwoodite. As these solids precipitate they can segregate from liquid by density contrasts, thus causing elemental fractionation which can be used to decipher timing of differentiation. Mineral/melt and metal/silicate equilibria in our lab have helped to better understand high pressure fractionation of isotopic parent/daughter pairs Hf/W, Mn/Cr, Pd/Ag, Pt/Os, Re/Os, and U/Pb, and their application to Earth, Moon and Mars. There remains great potential for multi-anvil experimentation to shed light on many pressure–dependent aspects of planetary evolution such as core formation, high pressure phase equilibria, redox equilibria, and volatile evolution and storage. References1. Leinenweber, K., et al.(2012) American Mineralogist,97, 353–368. 2.Righter, K., et al.(2020) Geochem. Persp. Lett.15, 1-6.3. Righter, K., et al.(2020) Met. Planet. Sci 55, 2741-2757.4. Righter, K., et al.(2020)Earth and Planetary Science Letters,552, 116590.
pressure↗
Gamma-ray continuum and line observations of SN 1987A
The Caltech gamma-ray imaging telescope observed the hard X-ray and gamma-ray emission from SN 1987A as it evolved between 1987 May and 1989 April, in a series of four balloon flights from Alice Springs, NT, Australia. Observations of the Crab Nebula and Pulsar provided in-flight data on pointing accuracy and instrument function for each flight. Results presented here include our measurements on November 18, 1987 (D268) and April 12, 1988 (D414) of both line emission at 847 and 1238 keV from the decay of Co-56, and Compton-scattered continuum above 50 keV. Upper limits for both line and continuum emission were obtained on May 20, 1987 (D86) and April 4, 1989 (D771). For the D268 and D414 continuum measurements, our results are best-fit by a differential power law of the form dN/dE = kE exp -gamma (sq cm s keV) for the energy range 50-800 keV. Our corresponding line measurements were fit with Gaussian profiles, containing additional terms for the underlying continuum. We compare our flux measurements and upper limits to those from other experiments and to predictions of theoretical models.
Palmer, D. M.↗
High Angular Resolution ALMA Images of Dust and Molecules in the SN 1987A Ejecta
We present high angular resolution (∼80 mas) ALMA continuum images of the SN1987A system, together with CO J = 21, J = 65, and SiO J = 54 to J = 76 images, which clearly resolve the ejecta (dust continuum and molecules) and ring (synchrotron continuum) components. Dust in the ejecta is asymmetric and clumpy, and overall the dust fills the spatial void seen in Hα images, filling that region with material from heavier elements. The dust clumps generally fill the space where CO J = 6 5 is fainter, tentatively indicating that these dust clumps and CO are locationally and chemically linked. In these regions, carbonaceous dust grains might have formed after dissociation of CO. The dust grains would have cooled by radiation, and subsequent collisions of grains with gas would also cool the gas, suppressing the CO J = 6 5 intensity. The data show a dust peak spatially coincident with the molecular hole seen in previous ALMA CO J = 2 1 and SiO J = 5 4 images. That dust peak, combined with CO and SiO line spectra, suggests that the dust and gas could be at higher temperatures than the surrounding material, though higher density cannot be totally excluded. One of the possibilities is that a compact source provides additional heat at that location. Fits to the far-infrared–millimeter spectral energy distribution give ejecta dust temperatures of 18–23 K. We revise the ejecta dust mass to Mdust = 0.2–0.4 Mfor carbon or silicate grains, or a maximum of <0.7 Mfor a mixture of grain species, using the predicted nucleosynthesis yields as an upper limit.
Interstellar dust↗
SN 1993J: A Type IIb supernova
The evolution of the bright Type II supernova discovered last year in M81, SN 1993J, is consistent with that expected for the explosion of a star which on the main sequence had a mass of 13-16 Solar Mass but which, owing to mass exchange with a binary companion (a intially approximately 3-5 AU, depending upon the actual presupernova radius and the masses of the two stars) lost almost all of its hydrogen-rich envelope during late helium burning. At the time of explosion, the helium core mass was 4.0 +/- 0.5 Solar Mass and the hydrogen envelope, 0.20 +/- 0.05 Solar Mass. The envelope was helium and nitrogen-rich (carbon-deficient) and the radius of the star, 4 +/- 1 x 10(exp 13) cm. The luminosity of the presupernova star was 3 + 1 x 10(exp 38) ergs/s, with the companion star contributing an additional approximately 10(exp 38) ergs/s. The star may have been a pulsating variable at the time of the explosion. For an explosion energy near 10(exp 51) ergs (KE at infinity) and an assumed distance of 3.3 Mpc, a mass of Ni-56 in the range 0.07 +/- 0.01 Solar Mass was produced and ejected. This presciption gives a light curve which compares favorably with the bolomatric observations. Color photometry is more restrictive and requires a model in which the hydrogen-envelope mass is low and the mixing of hydrogen inward has been small, but in which appreciable Ni-56 has been mixed outward into the helium and heavy-element core. It is possible to obtain good agreement with B and V light curves during the first 50 days, but later photometry, especially in bands other than B and V, will require a non-local thermo-dynamic equilibrium (LTE) spectral calculation for comparison. Based upon our model, we predict a flux of approximately 10(exp -5)(3.3 Mpc/D)(exp 2) photons/sq cm/s in the 847 keV line of CO-56 at peak during 1993 August. It may be easier to detect the Computonized continuum which peaks at a few times 10(exp -4) photons /s/sq cm/MeV at 40 keV a few months after the explosion (though neither of these signals were, or should have been, detected by the Compton Gamma-Ray observatory (CGRO). The presupernova star was filing its Roche lobe at the time of the explosion and thus its envelope was highly deformed (about 3:2). The companion star is presently embedded in the supernova, but should becopme visable at age 3 yr (perhaps earlier in the ultraviolet) when the supernova has faded below 10(exp 38) ergs/s. Indeed, if 'kicks' have not played an important role, it is still bound to the neutron star.
Woosley, S. E.↗