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1.
Materials (Basel) ; 17(11)2024 May 29.
Article in English | MEDLINE | ID: mdl-38893882

ABSTRACT

Rules that control the arrangement of chemical species within crystalline arrays of different symmetry and structural complexity are of fundamental importance in geoscience, material science, physics, and chemistry. Here, the volume of crystal phases is normalized by their ionic volume and an algebraic index that is based on their space-group and crystal site symmetries. In correlation with the number of chemical formula units Z, the normalized volumes exhibit upper and lower limits of possible structures. A bottleneck of narrowing limits occurs for Z around 80 to 100, but the field of allowed crystalline configurations widens above 100 due to a change in the slope of the lower limit. For small Z, the highest count of structures is closer to the upper limit, but at large Z, most materials assume structures close to the lower limit. In particular, for large Z, the normalized volume provides rather narrow constraints for the prediction of novel crystalline phases. In addition, an index of higher and lower complexity of crystalline phases is derived from the normalized volume and tested against key criteria.

2.
Science ; 376(6593): eabo2029, 2022 05 06.
Article in English | MEDLINE | ID: mdl-35536896

ABSTRACT

Walter et al. issue a number of critical comments on our report about the discovery of davemaoite to the end that they believe to show that our results do not provide compelling evidence for the presence of davemaoite in the type specimen and that the hosting diamond had formed in the lithosphere. Their claim is based on a misinterpretation of the diffraction data contained in the paper, an insufficient analysis of the compositional data that disregards the three-dimensional distribution of inclusions, and the arbitrary assumption that Earth's mantle shows no lateral variations in temperature, inconsistent with state-of-the-art assessments of mantle temperature variations and with their own published results.

3.
Science ; 374(6569): 891-894, 2021 Nov 12.
Article in English | MEDLINE | ID: mdl-34762475

ABSTRACT

Calcium silicate perovskite, CaSiO3, is arguably the most geochemically important phase in the lower mantle, because it concentrates elements that are incompatible in the upper mantle, including the heat-generating elements thorium and uranium, which have half-lives longer than the geologic history of Earth. We report CaSiO3-perovskite as an approved mineral (IMA2020-012a) with the name davemaoite. The natural specimen of davemaoite proves the existence of compositional heterogeneity within the lower mantle. Our observations indicate that davemaoite also hosts potassium in addition to uranium and thorium in its structure. Hence, the regional and global abundances of davemaoite influence the heat budget of the deep mantle, where the mineral is thermodynamically stable.

4.
Innovation (Camb) ; 2(2): 100117, 2021 May 28.
Article in English | MEDLINE | ID: mdl-34557764

ABSTRACT

Diamonds form in a variety of environments between subducted crust, lithospheric and deep mantle. Recently, deep source diamonds with inclusions of the high-pressure H2O-phase ice-VII were discovered. By correlating the pressures of ice-VII inclusions with those of other high-pressure inclusions, we assess quantitatively the pressures and temperatures of their entrapment. We show that the ice-VII-bearing diamonds formed at depths down to 800 ± 60 km but at temperatures 200-500 K below average mantle temperature that match the pressure-temperature conditions of decomposing dense hydrous mantle silicates. Our work presents strong evidence for coupled recycling of water and carbon in the deep mantle based on natural samples.

6.
Proc Natl Acad Sci U S A ; 117(21): 11217-11219, 2020 05 26.
Article in English | MEDLINE | ID: mdl-32393617

ABSTRACT

Understanding the timing and mechanisms of amino acid synthesis and racemization on asteroidal parent bodies is key to demonstrating how amino acids evolved to be mostly left-handed in living organisms on Earth. It has been postulated that racemization can occur rapidly dependent on several factors, including the pH of the aqueous solution. Here, we conduct nanoscale geochemical analysis of a framboidal magnetite grain within the Tagish Lake carbonaceous chondrite to demonstrate that the interlocking crystal arrangement formed within a sodium-rich, alkaline fluid environment. Notably, we report on the discovery of Na-enriched subgrain boundaries and nanometer-scale Ca and Mg layers surrounding individual framboids. These interstitial coatings would yield a surface charge state of zero in more-alkaline fluids and prevent assimilation of the individual framboids into a single grain. This basic solution would support rapid synthesis and racemization rates on the order of years, suggesting that the low abundances of amino acids in Tagish Lake cannot be ascribed to fluid chemistry.


Subject(s)
Amino Acids , Meteoroids , Sodium/chemistry , Water/chemistry , Amino Acids/biosynthesis , Amino Acids/chemical synthesis , British Columbia , Calcium/chemistry , Ferrosoferric Oxide/chemistry , Hydrogen-Ion Concentration , Lakes , Magnesium/chemistry , Stereoisomerism , Tomography/methods
7.
Nat Commun ; 8(1): 1230, 2017 11 01.
Article in English | MEDLINE | ID: mdl-29089493

ABSTRACT

Clay mineral-bearing locations have been targeted for martian exploration as potentially habitable environments and as possible repositories for the preservation of organic matter. Although organic matter has been detected at Gale Crater, Mars, its concentrations are lower than expected from meteoritic and indigenous igneous and hydrothermal reduced carbon. We conducted synthesis experiments motivated by the hypothesis that some clay mineral formation may have occurred under oxidized conditions conducive to the destruction of organics. Previous work has suggested that anoxic and/or reducing conditions are needed to synthesize the Fe-rich clay mineral nontronite at low temperatures. In contrast, our experiments demonstrated the rapid formation of Fe-rich clay minerals of variable crystallinity from aqueous Fe3+ with small amounts of aqueous Mg2+. Our results suggest that Fe-rich clay minerals such as nontronite can form rapidly under oxidized conditions, which could help explain low concentrations of organics within some smectite-containing rocks or sediments on Mars.

8.
Proc Natl Acad Sci U S A ; 113(26): 7077-81, 2016 06 28.
Article in English | MEDLINE | ID: mdl-27298357

ABSTRACT

We designed a plate impact shock recovery experiment to simulate the starting materials and shock conditions associated with the only known natural quasicrystals, in the Khatyrka meteorite. At the boundaries among CuAl5, (Mg0.75Fe(2+) 0.25)2SiO4 olivine, and the stainless steel chamber walls, the recovered specimen contains numerous micron-scale grains of a quasicrystalline phase displaying face-centered icosahedral symmetry and low phason strain. The compositional range of the icosahedral phase is Al68-73Fe11-16Cu10-12Cr1-4Ni1-2 and extends toward higher Al/(Cu+Fe) and Fe/Cu ratios than those reported for natural icosahedrite or for any previously known synthetic quasicrystal in the Al-Cu-Fe system. The shock-induced synthesis demonstrated in this experiment reinforces the evidence that natural quasicrystals formed during a shock event but leaves open the question of whether this synthesis pathway is attributable to the expanded thermodynamic stability range of the quasicrystalline phase at high pressure, to a favorable kinetic pathway that exists under shock conditions, or to both thermodynamic and kinetic factors.

9.
Science ; 346(6213): 1100-2, 2014 Nov 28.
Article in English | MEDLINE | ID: mdl-25430766

ABSTRACT

Meteorites exposed to high pressures and temperatures during impact-induced shock often contain minerals whose occurrence and stability normally confine them to the deeper portions of Earth's mantle. One exception has been MgSiO3 in the perovskite structure, which is the most abundant solid phase in Earth. Here we report the discovery of this important phase as a mineral in the Tenham L6 chondrite and approved by the International Mineralogical Association (specimen IMA 2014-017). MgSiO3-perovskite is now called bridgmanite. The associated phase assemblage constrains peak shock conditions to ~ 24 gigapascals and 2300 kelvin. The discovery concludes a half century of efforts to find, identify, and characterize a natural specimen of this important mineral.

10.
Astrobiology ; 13(11): 1049-64, 2013 Nov.
Article in English | MEDLINE | ID: mdl-24283927

ABSTRACT

Fumaroles represent a very important potential habitat on Mars because they contain water and nutrients. Global deposition of volcanic sulfate aerosols may also have been an important soil-forming process affecting large areas of Mars. Here we identify alteration from the Senator fumarole, northwest Nevada, USA, and in low-temperature environments near the fumarole to help interpret fumarolic and acid vapor alteration of rocks and soils on Mars. We analyzed soil samples and fluorapatite, olivine, and basaltic glass placed at and near the fumarole in in situ mineral alteration experiments designed to measure weathering under natural field conditions. Using synchrotron X-ray diffraction, we clearly observe hydroxyl-carbonate-bearing fluorapatite as a fumarolic alteration product of the original material, fluorapatite. The composition of apatites as well as secondary phosphates has been previously used to infer magmatic conditions as well as fumarolic conditions on Mars. To our knowledge, the observations reported here represent the first documented instance of formation of hydroxyl-carbonate-bearing apatite from fluorapatite in a field experiment. Retreat of olivine surfaces, as well as abundant NH4-containing minerals, was also characteristic of fumarolic alteration. In contrast, alteration in the nearby low-temperature environment resulted in formation of large pits on olivine surfaces, which were clearly distinguishable from the fumarolic alteration. Raman signatures of some fumarolically impacted surfaces are consistent with detection of the biological molecules chlorophyll and scytenomin, potentially useful biosignatures. Observations of altered minerals on Mars may therefore help identify the environment of formation and understand the aqueous history and potential habitability of that planet.


Subject(s)
Apatites/chemistry , Extraterrestrial Environment , Iron Compounds/chemistry , Magnesium Compounds/chemistry , Mars , Silicates/chemistry , Geological Phenomena , Glass/chemistry , Life
11.
Proc Natl Acad Sci U S A ; 106(33): 13691-5, 2009 Aug 18.
Article in English | MEDLINE | ID: mdl-19667178

ABSTRACT

We observed micrometer-sized grains of wadsleyite, a high-pressure phase of (Mg,Fe)(2)SiO(4,) in the recovery products of a shock experiment. We infer these grains crystallized from shock-generated melt over a time interval of <1 micros, the maximum time over which our experiment reached and sustained pressure sufficient to stabilize this phase. This rapid crystal growth rate (approximately 1 m/s) suggests that, contrary to the conclusions of previous studies of the occurrence of high-pressure phases in shock-melt veins in strongly shocked meteorites, the growth of high-pressure phases from the melt during shock events is not diffusion-controlled. Another process, such as microturbulent transport, must be active in the crystal growth process. This result implies that the times necessary to crystallize the high-pressure phases in shocked meteorites may correspond to shock pressure durations achieved on impacts between objects 1-5 m in diameter and not, as previously inferred, approximately 1-5 km in diameter. These results may also provide another pathway for syntheses, via shock recovery, of some high-value, high-pressure phases.


Subject(s)
Metals/chemistry , Silicates/chemistry , Silicon/chemistry , Solar System , Crystallization , Light , Microscopy, Electron, Scanning/methods , Pressure , Scattering, Radiation , Software , Spectrophotometry, Infrared/methods , Synchrotrons , Temperature , X-Ray Diffraction
12.
J Chem Phys ; 128(6): 064510, 2008 Feb 14.
Article in English | MEDLINE | ID: mdl-18282059

ABSTRACT

Ice VII was examined over the entire range of its pressure stability by a suite of x-ray diffraction techniques in order to understand a number of unexplained characteristics of its high-pressure behavior. Axial and radial polycrystalline (diamond anvil cell) x-ray diffraction measurements reveal a splitting of diffraction lines accompanied by changes in sample texture and elastic anisotropy. In situ laser heating of polycrystalline samples resulted in the sharpening of diffraction peaks due to release of nonhydrostatic stresses but did not remove the splitting. Radial diffraction measurements indicate changes in strength of the material at this pressure. Taken together, these observations provide evidence for a transition in ice VII near 14 GPa involving changes in the character of the proton order/disorder. The results are consistent with previous reports of changes in phase boundaries and equation of state at this pressure. The transition can be interpreted as ferroelastic with the appearance of spontaneous strain that vanishes at the hydrogen bond symmetrization transition near 60 GPa.

13.
J Synchrotron Radiat ; 12(Pt 5): 626-31, 2005 Sep.
Article in English | MEDLINE | ID: mdl-16120986

ABSTRACT

Among the many problems associated with high-pressure X-ray diffraction from polycrystalline samples in the diamond-anvil cell are strain and preferred orientation. A method is presented for efficiently reducing preferred orientation of powder samples compressed in diamond-anvil cells to pressures in excess of 20 GPa. This method may be successfully applied to samples of yield strength higher than alkalihalides. In addition, the problem of strain is discussed using ice-VII as an example and as an illustration of the importance of laser heating as a method of minimizing strain.

14.
J Chem Phys ; 123(2): 24703, 2005 Jul 08.
Article in English | MEDLINE | ID: mdl-16050762

ABSTRACT

We report a novel crystalline carbon-cage structure synthesized from laser-driven shock wave loading of a graphite-copper mixture to about 14+/-2 GPa and 1000 +/- 200 K. Quite unexpectedly, it can be structurally related to an extremely compressed three-dimensional C60 polymer with random displacement of C atoms around average positions equivalent to those of distorted C60 cages. Thus, the present carbon-cage structure represents a structural crossing point between graphite interlayer bridging and C60 polymerization as the two ways of forming diamond from two-dimensional and molecular carbon.

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