基于紧束缚分子动力学模型的Na4,Na8和Na20团簇结构及热力学性质研究

利用距离相关的紧束缚的分子动力学模型（DDTB－MD），通过提取不同温度下的势能、构型、无单位键长涨落平均位移、扩散系数、围绕质心的径向分布等参量，系统的研究了菱形结构和T形结构的Na4、Td结构和D2d结构的Na8，以及Na20的热力学的性质。对于Na4，比较了金属团簇Na4的菱形结构和T形结构两种异构体之间热力学性质的异同。发现在团簇温度升高的过程中，两种异构体都会发生从类固到类液的相变。T形结构的Na4熔点要比菱形结构的低。在相变的过程中都会发生赝转动和异构化。还发现了赝转动的判据不仅仅只是温度，还包括无单位键长涨落的δ值。菱形结构的Na4在200K左右不一定会发生赝转动，只有观察到温度处于200K左右，δ值≥0.08的时候，赝转动则必然会观察到。菱形结构Na4的赝转动过程中会发现T形结构的异构化，但其维持时间很短，不稳定，很快又转变为菱形结构。而T形结构在170K就能观察到异构化和赝转动的发生，在这个温度下会不断的在菱形与T型之间发生异构，而处于菱形结构的时间要比T型长的多。表现为菱形结构的稳定性要大于T型。对于Na8的两种不同的异构体（分别为Td结构和D2d结构），发现尽管两个异构体的基态能量很接近，但他们的稳定性、熔化过程的热力学性质等有着很大的差别，这也反映了它们在几何结构上的差别。对称性强的Td结构更紧密，在熔化过程中表现出更高的稳定性，具有较高的熔点，具有类晶体的性质.对称性弱的D2d结构则具有较低的熔点，很宽的熔化温度范围，具有类似非晶体的性质. 再比较了基态结构下的Na8和Na20。通过提取对不同的子系统在不同温度下的无单位键长涨落等参数，发现金属原子团簇Na20在熔化过程中表现出了并不像通常金属团簇那样的表面先熔化，而是从内部开始先熔化的奇异特性

几何结构对Na_8团簇熔化过程的影响

运用距离相关紧密结合的分子动力学模型,对金属原子团簇Na8的两种不同的异构体进行了数值模拟.根据零温下基态结构中不同原子到质心的不同距离,把Na8的两种异构体分为多个子系统.分别提取各个子系统在不同温度下的围绕质心的径向分布、无单位键长涨落、平均位移、扩散系数,发现尽管两个异构体的基态能量很接近,但他们的稳定性、熔化过程的热力学性质等有着很大的差别,这也反映了它们在几何结构上的差别.

钠原子团簇相变的多极形变特征

运用距离相关紧密结合的分子动力学模型 ,通过无量纲的形变参数S1对简单金属原子团簇Na4 、Na8、Na14 和Na2 0 相变时的多极形变特征进行了分析 ,发现S1可以用作表征团簇形变的灵敏探针。

不同初始温度时Na_8+Na_8团簇碰撞动力学研究

采用距离相关紧束缚的分子动力学模型 ,在不同初始温度T0 =0 .0 2K、50K、10 0K、2 0 0K、30 0K、4 0 0K时 ,对Na8+Na8在质心系轰击能量为 0 .0 12 5eV/n的中心碰撞时的反应动力学进行了研究。发现团簇碰撞动力学与初始温度密切相关。在T0 <10 0K时 ,初始温度不影响反应动力学 ,而在T0 =4 0 0K时将对反应动力学有强烈影响。

High-temperature induced dehydration, phase transition and exsolution in amicite: A single-crystal X-ray study

Temperature dependent single-crystal X-ray data were collected on amicite K4Na4(Al8Si8O32)·11H2O from Kola Peninsula (Russia) in steps of 25 °C from room temperature to 175 °C and of 50 °C up to 425 °C. At room temperature amicite has space group I2 with a = 10.2112(1), b = 10.4154(1), c = 9.8802(1) Å, β = 88.458(1)°, V = 1050.416(18) Å3. Its crystal structure is based on a Si–Al ordered tetrahedral framework of the GIS type with two systems of eight-membered channels running along the a and c axes. Extraframework K and Na cations are ordered at two fully occupied sites. Above 75 °C amicite was found to partly dehydrate into two separate but coherently intergrown phases, both of space group I2/a, one K-rich ∼K8(Al8Si8O32) ·4H2O (at 75 °C: a = 10.038(2), b = 9.6805(19), c = 9.843(2) Å, β = 89.93(3)°, V = 956.5(3) Å3) and the other Na-rich ∼Na8(Al8Si8O32)·2H2O (at 75 °C: a = 9.759(2), b = 8.9078(18), c = 9.5270(19) Å, β = 89.98(3)°, V = 828.2(3) Å3). Upon further heating above 75 °C the Na- and K-phases lost remaining H2O with only minor influence on the framework structure and became anhydrous at 175 °C and 375 °C, respectively. The two anhydrous phases persisted up to 425 °C. Backscattered electron images of a heated crystal displayed lamellar intergrowth of the K- and Na-rich phases. Exposed to ambient humid conditions K- and Na-rich phases rehydrated and conjoined to the original one phase I2 structure.

Geochemistry of dikes and lavas from the north wall of the Hess Deep Rift

An investigation of ~1-m.y.-old dikes and lavas from the north wall of the Hess Deep Rift (2°15'N, 101°30'W) collected during Alvin expeditions provides a detailed view of the evolution of fast spreading oceanic crust. The study area encompasses 25 km of an east-west flow line, representing ~370,000 years of crustal accretion at the East Pacific Rise. Samples analyzed exhibit depleted incompatible trace element abundances and ratios [(La/Sm)N < 1]. Indices of fractionation (MgO), and incompatible element ratios (La/Sm, Nb/Ti) show no systematic trends along flow line. Rather, over short (<4 m) and long (~25 km) distances, significant variations are observed in major and trace element concentrations and ratios. Modeling of these variations attests to the juxtaposition of dikes of distinct parental magma compositions. These findings, combined with studies of segmentation of the subaxial magma chamber and lateral magma transport in dikes along rift-dominated systems, suggest a more realistic model of the magmatic system underlying the East Pacific Rise relative to the commonly assumed twodimensional model. In this model, melts from a heterogeneous mantle feed distinct portions of a segmented axial magma reservoir. Dikes emanating from these distinct reservoirs transport magma along axis, resulting in interleaved dikes and host lavas with different evolutionary histories. This model suggests the use of axial or flow line lava compositions to infer the evolution of axial magma chambers should be approached with caution because dikes may never erupt lava or may transport magma significant distances along axis and erupt lavas far from their axial magma chamber of origin.

Geochemistry of volcanic glass from ODP holes 129-801C and 185-801C in the western Pacific

Major element chemistry of basalt from the southern East Pacific Rise (EPR) is different from that of the EPR at the time of the formation of the Pacific Plate at 170 Ma.Glass recovered from Jurassic age (170 Ma) Pacific ocean crust (Bartolini and Larson, 2001, doi:10.1130/0091-7613(2001)029<0735:PMATPS>2.0.CO;2) at Ocean Drilling Program Hole 801C records higher Fe8 (10.77 wt%) and marginally lower Na8 (2.21 wt%) compared to the modern EPR, suggesting deeper melting and a temperature of initial melting that was 60°C hotter than today.Trace element ratios such as La/Sm and Zr/Y, on the other hand, show remarkable similarities to the modern southern EPR, indicating that Site 801 was not generated on a hotspot-influenced ridge and that mantle composition has changed little in the Pacific over the past 170 Ma. Our results are consistent with the observation that mid-ocean ridge basalts (MORBs) older than 80 Ma were derived by higher temperature melting than are modern MORBs (Humler et al., 1999, doi:10.1016/S0012-821X(99)00218-6), which may have been a consequence of the Cretaceous superplume event in the Pacific.Site 801 predates the formation of Pacific oceanic plateaus and 801C basalt chemistry indicates that higher temperatures of mantle melting beneath Pacific ridges preceded the initiation of the superplume.