# Ab initio chemical potentials of solid and liquid solutions and the chemistry of the Earth's core

@article{Alf2002AbIC, title={Ab initio chemical potentials of solid and liquid solutions and the chemistry of the Earth's core}, author={Dario Alf{\'e} and Michael J. Gillan and Geoffrey D. Price}, journal={Journal of Chemical Physics}, year={2002}, volume={116}, pages={7127-7136} }

A general set of methods is presented for calculating chemical potentials in solid and liquid mixtures using ab initio techniques based on density functional theory (DFT). The methods are designed to give an ab initio approach to treating chemical equilibrium between coexisting solid and liquid solutions, and particularly the partitioning ratios of solutes between such solutions. For the liquid phase, the methods are based on the general technique of thermodynamic integration, applied to… Expand

#### 95 Citations

Theory and Practice – The Ab Initio Treatment of High-Pressure and -Temperature Mineral Properties and Behavior

- Chemistry
- 2007

Ab initio techniques, mainly based on the implementation of quantum mechanics known as density functional theory (DFT), are now widely used in the investigation of the high-pressure and -temperature… Expand

First-principles simulations of direct coexistence of solid and liquid aluminum

- Materials Science, Physics
- 2003

First-principles calculations based on density-functional theory, with generalized gradient corrections and ultrasoft pseudopotentials, have been used to simulate solid and liquid aluminum in direct… Expand

The Ab Initio Treatment of High-Pressure and High-Temperature Mineral Properties and Behavior

- Chemistry
- 2015

Ab initio techniques, mainly based on the implementation of quantum mechanics known as density functional theory (DFT), have now become widely used in the investigation of the high-pressure and… Expand

Thermodynamics from first principles : temperature and composition of the Earth s core

- 2003

We summarize the main ideas used to determine the thermodynamic properties of pure systems and binary alloys from first principles calculations. These are based on the ab initio calculations of free… Expand

Thermodynamics from first principles: temperature and composition of the Earth’s core

- Chemistry
- Mineralogical Magazine
- 2003

Abstract We summarize the main ideas used to determine the thermodynamic properties of pure systems and binary alloys from first principles calculations. These are based on the ab initio calculations… Expand

Ab initio modeling of alloy phase equilibria

- Materials Science
- 2007

In this chapter we provide an overview of the methodologies underlying first-principles (or ab initio) calculations of alloy phase stability, and provide examples intended to illustrate their… Expand

Ni partitioning between metal and silicate melts: An exploratory ab initio molecular dynamics simulation study

- Geology
- 2017

Abstract Element partitioning is a key geochemical process. While partition coefficients between phases including melts have been measured in many experimental studies, new insight into the… Expand

Absolute rate of thermal desorption from first-principles simulation.

- Chemistry, Medicine
- Journal of physics. Condensed matter : an Institute of Physics journal
- 2006

We present a technique for computing by first-principles simulation the absolute desorption rate γ of adsorbate molecules from a surface for any coverage and temperature. The technique is valid when… Expand

Ab initio study of the phase separation of argon in molten iron at high pressures

- Materials Science
- 2006

[1] Using first-principles molecular dynamics (MD) simulations, we study the solubility of argon in molten iron at high pressures and temperatures. In particular we explore whether the low pressure… Expand

Two-phase simulation of the crystalline silicon melting line at pressures from -1 to 3 GPa.

- Medicine, Chemistry
- The Journal of chemical physics
- 2012

A two-phase molecular dynamics method is applied to obtain temperature, pressure, and densities of solid and liquid phases on the melting line and a special procedure is used to ensure the strict control of the two- phase equilibrium in the simulation cell. Expand

#### References

SHOWING 1-10 OF 46 REFERENCES

Thermodynamic Stability of Fe/O Solid Solution at Inner‐Core Conditions

- Materials Science, Physics
- 2000

We present a new technique which allows the fully ab initio calculation of the chemical potential of a substitutional impurity in a high-temperature crystal, including harmonic and anharmonic lattice… Expand

Ab initio determination of the melting point of aluminum by thermodynamic integration

- Chemistry
- 2000

The melting point of aluminum has been obtained in an ab initio molecular dynamics calculation by determination of the free energies of the solid and liquid phases as a function of temperature along… Expand

Thermodynamics of hexagonal-close-packed iron under Earth’s core conditions

- Physics
- 1999

The free energy and other thermodynamic properties of hexagonal-close-packed iron are calculated by direct ab initio methods over a wide range of pressures and temperatures relevant to the Earth’s… Expand

Free-energy calculations in solids from first-principles molecular dynamics: Vacancy formation in sodium.

- Materials Science, Medicine
- Physical review. B, Condensed matter
- 1995

Thermodynamic integration methods are applied to obtain the classical free energy of solids via first-principles simulations based upon the Car-Parrinello strategy and it is found that specific techniques have to be used to ensure canonical sampling, particularly for the case of the perfect-crystal calculations. Expand

Oxygen in the Earth's core: a first-principles study

- Materials Science, Physics
- 1999

Abstract 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… Expand

Composition and temperature of the Earth's core constrained by combining ab initio calculations and seismic data

- Geology
- 2002

It is shown how ab initio techniques based on density functional theory can be used to calculate the chemical potentials of the leading candidate impurity elements (S, O and Si) in the Earth’s solid… Expand

Ab initio molecular dynamics study of first-order phase transitions: melting of silicon.

- Materials Science, Medicine
- Physical review letters
- 1995

It is shown that properties like the specific entropy, the specific volume, or the heat capacity of a solid and a liquid can be calculated accurately and this greatly extends the range of first-principles predictions of materials properties. Expand

First-principles simulations of liquid Fe-S under Earth's core conditions

- Materials Science, Physics
- 1998

First-principles electronic structure calculations, based upon density functional theory within the generalized gradient approximation and ultrasoft Vanderbilt pseudopotentials, have been used to… Expand

Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set

- Materials Science
- 1996

We present a detailed description and comparison of algorithms for performing ab-initio quantum-mechanical calculations using pseudopotentials and a plane-wave basis set. We will discuss: (a) partial… Expand

Structure and dynamics of liquid iron under Earth’s core conditions

- Physics
- 2000

First-principles molecular-dynamics simulations based on density-functional theory and the projector augmented wave (PAW) technique have been used to study the structural and dynamical properties of… Expand