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Stephan Lowitzer Dan J. Wilson Björn Winkler Victor Milman Julian D. Gale 《Physics and Chemistry of Minerals》2008,35(3):129-135
Knowledge of the defect properties of Lunar and Mercurian minerals has recently become important, with the advent of models
which attempt to explain the formation of the thin exosphere of these celestial bodies. Here, we have calculated the formation
energies of sodium and oxygen vacancies in the mineral albite (NaAlSi3O8), as well as the Schottky defect energy for the removal of a Na2O unit. We have employed both the supercell and Mott–Littleton approaches, using Kohn–Sham density functional theory and classical
interatomic potential methods. As well as reporting the defect energies and structures, we comment upon the relative merits
of the methods used. 相似文献
2.
Equilibrium isotope fractionation of thallium(Tl) includes the traditional mass-dependent isotope fractionation effect and the nuclear volume effect(NVE). The NVE dominates the overall isotope fractionation, especially at high temperatures. Heavy Tl isotopes tend to be enriched in oxidized Tl^3+-bearing species. Our NVE fractionation results of oxidizing Tl^+ to Tl^3+ can explain the positive enrichments observed in ferromanganese sediments. Experimental results indicate that there could be0.2–0.3 e-unit fractionation between sulfides and silicates at 1650 ℃. It is consistent with our calculation results,which are in the range of 0.17–0.38 e-unit. Importantly,Tl’s concentration in the bulk silicate Earth(BSE) can be used to constrain the amount of materials delivered to Earth during the late veneer accretion stage. Because the Tl concentration in BSE is very low and its Tl isotope composition is similar with that of chondrites, suggesting either no Tl isotope fractionation occurred during numerous evaporation events, or the Tl in current BSE was totally delivered by late veneer. If it is the latter, the Tl-contentbased estimation could challenge the magnitude of late veneer which had been constrained by the amount of highly siderophile elements in BSE. Our results show that the lateaccreted mass is at least five-times larger than the previously suggested magnitude, i.e., 0.5 wt% of current Earth’s mass. The slightly lighter 205 Tl composition of BSE relative to chondrites is probable a sign of occurrence of Tlbearing sulfides, which probably were removed from the mantle in the last accretion stage of the Earth. 相似文献
3.
R. Bianchi A. Forni F. Cámara R. Oberti H. Ohashi 《Physics and Chemistry of Minerals》2007,34(8):519-527
The synthetic LiGaSi2O6 clinopyroxene is monoclinic C2/c at room-T. Its experimental electron density, ρ(r), has been derived starting from accurate room-T single-crystal diffraction data. Topological analysis confirms an intermediate ionic-covalent character for Si–O bonding,
as found by previous electron-density studies on other silicates such as diopside, coesite and stishovite. The non-bridging
Si–O bonds have more covalent character than the bridging ones. The Ga–O bonds have different bonding characters, the Ga–O2
bond being more covalent than the two Ga–O1 bonds. Li–O bonds are classified as pure closed-shell ionic interactions. Similar
to spodumene (LiAlSi2O6), Li has sixfold coordination, but the bond critical points associated to the two longest bonds are characterized by very
low electron density values. Similar to what previously found in spodumene and diopside, O···O interactions were detected
from the topological analysis of ρ(r), and indicate a cooperative interaction among the lone pairs of neighbouring oxygen atoms. In particular, this kind of interaction
has been obtained for the O1···O1 edge shared between two Ga octahedra. Integration over the atomic basins gives net charges
of −1.39(10), 2.82(10), 1.91(10) and 0.82(8) e for O (averaged), Si, Ga and Li atoms, respectively. Periodic Hartree–Fock
and DFT calculations confirm the results obtained by multipole refinement of the experimental data. Moreover, the theoretical
topological properties of the electron density distribution on the Si2O6 group are very similar to those calculated for spodumene.
Electronic supplementary material The online version of this article (doi:) contains supplementary material, which is available to authorized users. 相似文献
4.
高温高压下黄铁矿热力学性质的第一性原理研究 总被引：1，自引：0，他引：1
黄铁矿是自然界中分布最为广泛的硫化物矿物,同时也是重要的造矿矿物,在金属矿床、沉积岩、变质岩、花岗岩、基性-超基性岩浆岩、以及地幔岩中都有大量出现。因此,研究黄铁矿在不同温度压力下的热力学性质可以为深入探讨与黄铁矿有关的成岩、成矿、成藏问题提供有用的矿物学依据。本文利用基于密度泛函微扰理论的第一性原理方法,采用准谐近似计算了黄铁矿在高温高压下的热力学性质。我们计算的黄铁矿的晶格常数、零压下的体积模量及其对压力的导数与前人的实验及理论计算结果吻合得很好,零压下等压热容和熵随温度的变化与实验结果有很好的一致性。尤其是,本文计算了直至2500K、100GPa的高温高压下黄铁矿的等温体积模量、热膨胀系数、热容和熵等热力学性质。这为在有硫参与的情况下,人们开展下地壳-岩石圈地幔深度的地球动力学模拟和建立地球物理模型提供了有用的信息。 相似文献
5.
Dario Alf G. David Price Michael J. Gillan 《Physics of the Earth and Planetary Interiors》1999,110(3-4):191-210
First-principles electronic structure calculations based on DFT have been used to study the thermodynamic, structural and transport properties of solid solutions and liquid alloys of iron and oxygen at Earth's core conditions. Aims of the work are to determine the oxygen concentration needed to account for the inferred density in the outer core, to probe the stability of the liquid against phase separation, to interpret the bonding in the liquid, and to find out whether the viscosity differs significantly from that of pure liquid iron at the same conditions. It is shown that the required concentration of oxygen is in the region 25–30 mol%, and evidence is presented for phase stability at these conditions. The Fe/O bonding is partly ionic, but with a strong covalent component. The viscosity is lower than that of pure liquid iron at Earth's core conditions. It is shown that earlier first-principles calculations indicating very large enthalpies of formation of solid solutions may need reinterpretation, since the assumed crystal structures are not the most stable at the oxygen concentration of interest. 相似文献
6.
Previous theoretical studies have found that the concentration variations within a certain range have a prominent effect on inter-mineral equilibrium isotope fractionation(10^3 lna).Based on the density functional theory,we investigated how the average Ca–O bond length and the reduced partition function ratios(10^3 lnb)and103lna of 44 Ca/40 Ca in forsterite(Fo)are affected by its Ca concentration.Our results show that Ca–O bond length in forsterite ranges from 2.327 to 2.267 A with the Ca/(Ca+Mg)varying between a narrow range limited by an upper limit of 1/8 and a lower limit of 1/64.However,outside this narrow range,i.e.,Ca/(Ca+Mg)is lower than1/64 or higher than 1/8,Ca–O bond length becomes insensitive to Ca concentration and maintains to be a constant.Because the 10^3 lnb is negatively correlated with Ca–O bond length,the 10^3lnb significantly increases with decreasing Ca/(Ca+Mg)when 1/64相似文献
7.
J.-P. Crocombette 《Physics and Chemistry of Minerals》1999,27(2):138-143
We present a numerical study of point defects in crystalline zircon (ZrSiO4). Vacancies and interstitials of all the constituents of zircon have been considered. For each defect, the structure and
the formation energies have been calculated. Calculations, using the supercell method, are based on the Density Functional
Theory in the Local Density Approximation. Empirical potentials have also been considered for comparison with electronic structure
results. We find a formation energy for the oxygen interstitial of 1.7 eV. This value is compatible with the experimental
activation energy for oxygen diffusion in zircon, which proves an interstitial mechanism for the diffusion of oxygen in zircon.
For all other defects the calculated formation energies lead to negligible thermal concentration at equilibrium.
Received: 8 January 1999 / Revised, accepted: 14 May 1999 相似文献
8.
以盐湖卤水为原料提取并制备Li2CO3的过程中,共存离子对其结晶过程影响较大,尤其我国西藏盐湖卤水为原料制备碳酸锂的原料中,K/Li约为0.3左右,所以研究K+对Li2CO3晶体的影响具有重要意义。通过实验和计算模拟相结合研究不同K/Li条件下K+对Li2CO3晶体的影响程度,建立晶体中K+含量与比表面积关联式。实验结果表明,K+的存在对Li2CO3的高品质性影响较大,且随着钾离子含量增加,晶体比表面积增大易于吸附杂质离子,表面粗糙度增强,且K+存在对碳酸锂晶体的收率影响较大,而当K/Li控制在0.1以内时,K+对碳酸锂晶体的影响相对较小。通过第一性原理计算,计算并分析了K掺入碳酸锂晶体中的几何结构、缺陷形成能及态密度,结果表明K原子在碳酸锂晶体中更易替代晶体中的Li原子,K原子的掺入对碳酸锂晶体的晶格参数以及电子结构性质的影响较小。对西藏盐湖高效提锂和制备高附加值碳酸锂晶体提供了理论依据。 相似文献
9.
以盐湖卤水为原料提取并制备Li2CO3的过程中,共存离子对其结晶过程影响较大,尤其西藏盐湖卤水为原料制备碳酸锂的原料中,K/Li约为0.3左右,所以研究K+对Li2CO3晶体的影响具有重要意义。本研究通过实验和计算模拟相结合研究不同K/Li条件下K+对Li2CO3晶体的影响程度,建立晶体中K+含量与比表面积关联式。实验结果表明,K+的存在对Li2CO3的高品质性影响较大,且随着钾离子含量增加,晶体比表面积增大易于吸附杂质离子,表面粗糙度增强,且K+存在对碳酸锂晶体的收率影响较大,而当K/Li控制在0.1以内时,K+对碳酸锂晶体的影响相对较小;通过第一性原理计算,计算并分析了K掺入碳酸锂晶体中的几何结构、缺陷形成能及态密度,结果表明K原子在碳酸锂晶体中更易替代晶体中的Li原子,且K原子的掺入对碳酸锂晶体的晶格参数以及电子结构性质的影响较小。本文对西藏盐湖高效提锂和制备高附加值碳酸锂晶体提供理论依据。 相似文献
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