DOI: 10.5281/zenodo.3527985
title: Speciation data for "Pressure-induced coordination changes in a pyrolitic silicate melt from ab initio molecular dynamics simulations"

description: With <em>ab initio</em> molecular dynamics simulations on pyrolite melt, we examine the detailed changes in elemental coordination as a function of pressure and temperature. We consider the average coordination as well as the proportion and distribution of coordination environments at pressures and temperatures encompassing the conditions at which molten silicates may exist in present-day Earth and those of the Early Earth's magma ocean. At ambient pressure and 2000 K, we find that the average coordination of cations with respect to oxygen is 4.0 for Si-O, 4.0 for Al-O, 3.7 for Fe-O, 4.6 for Mg-O, 5.9 for Na-O and 6.2 for Ca-O. Although the coordination for iron with respect to oxygen is underestimated, the coordination number for all other cations are consistent with experiments. At the base of the upper mantle (~15 GPa and 2000 K), the average coordination for Si-O remains at 4.0, but increases to 4.1 for Al-O, 4.2 for Fe-O, 4.9 for Mg-O, 8.0 for Na-O and 6.8 for Ca-O. The coordination environment for Na-O remains approximately constant up to core-mantle boundary conditions (135 GPa and 4000 K), but increases to about 6 for Si-O, 6.5 for Al-O, 6.5 for Fe-O, 8 for Mg-O, 9.5 for Ca-O. Our results have implications for melt properties, such as viscosity, transport coefficients, thermal conductivities and electrical conductivities, and will help interpret experimental results on silicate glasses. Detailed speciation statistics for pyrolite melt were determined using <em>a</em><em>b initio</em> molecular dynamics simulations with the Vienna Ab Initio Simulation Package (VASP) (Kresse and Furthmuller, 1996). Simulations were performed with a time step of 0.5-2 femtoseconds for 10-50 picoseconds, depending on the temperature and density. The composition of the Bulk Silicate Earth was modeled with a pyrolite melt with the stoichiometry NaCa<sub>2</sub>Fe<sub>4</sub>Mg<sub>30</sub>Al<sub>3</sub>Si<sub>24</sub>O<sub>89</sub>. Bond distances were determined from the pair distribution functions, which describe the probability of finding an atom type at a given distance from the reference atom. We used the first peak in the pair distribution function to approximate the average bond length; the distance at which the first minimum occurs marks the radius of the first coordination sphere of atoms that are directly bonded to the reference atom. We used this value to define the bond criterion between two atom types. Additional computational details can be found in the manuscript.
description: In this dataset, the data is sorted first by temperature (in folders labeled as 2000K, 3000K...) and then by cation-oxygen pairs (in folders labeled as SiO, MgO...). Each file name contains the lattice parameter (for example, "a13.0" signifies a cell length of 13 Angstroms). There are two file types, "stat.dat" and "popul.dat" for the summarized statistics and detailed population files, respectively. In the stat.dat file, the first column signifies the cluster type (SiO_4, Si_O5...), the second column indicates the total (summed) length of time in femtoseconds that they existed for, the third column is the relative proportions (for example, 0.6 SiO_4 and 0.4 Si_O5 would mean that 60% of the silicon is fourfold coordinated and 40% is fivefold coordinated), the fourth column is the number of atoms in the cluster (e.g., SiO_4 contains five atoms). The popul.dat file contains a column with each individual species (SiO_4, Si_O5...), the time at which the species formed in femtoseconds, the time at which the species died in femtoseconds and the lifetime or duration of that species' existence (i.e., the end time minus the start time), and finally, the atom numbers for identity purposes. Corresponding pressures and pressure errors are found in the files within each temperature folder, labeled as "Pressures_2000K.dat" for example. The first column is the cell length in Angstroms, the second column is the calculated pressure in gigapascals and the third column is the standard deviation in gigapascals.