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S. I. Simak

Publications and source records attributed to S. I. Simak.

12 recordsLinked to original sources
arXiv2019

Impact of anharmonicity on sound wave velocities at extreme conditions

Theoretical calculations of sound-wave velocities of materials at extreme conditions are of great importance to various fields, in particular geophysics. For example, the seismic data on sound-wave propagation through the solid iron-rich Earth's inner core have been the main source for elucidating its properties and building models. As the laboratory experiments at very high temperatures and pressures are non-trivial, ab initio predictions are invaluable. The latter, however, tend to disagree with experiment. We notice that many attempts to calculate sound-wave velocities of matter at extreme conditions in the framework of quantum-mechanics based methods have not been taking into account the effect of anharmonic atomic vibrations. We show how anharmonic effects can be incorporated into ab initio calculations and demonstrate that in particular they might be non-negligible for iron in Earth's core. Therefore, we open an avenue to reconcile experiment and ab initio theory.

cond-mat.mtrl-sci↗
arXiv2019

Superionic-like diffusion in an elemental crystal: bcc Titanium

Recent theoretical investigations [Belonoshko et al. Nature Geoscience 10, 312 (2017)] revealed occurrence of concerted migration of several atoms in bcc Fe at inner-core temperatures and pressures. Here, we combine first-principles and semi-empirical atomistic simulations to show that a diffusion mechanism analogous to the one predicted for bcc iron at extreme conditions is also operative and of relevance for the high-temperature bcc phase of pure Ti at ambient pressure. The mechanism entails a rapid collective movement of numerous (from two to dozens) neighbors along tangled closed-loop paths in defect-free crystal regions. We argue that this phenomenon closely resembles the diffusion behavior of superionics and liquid metals. Furthermore, we suggest that concerted migration is the atomistic manifestation of vanishingly small w-mode phonon frequencies previously detected via neutron scattering and the mechanism underlying anomalously large and markedly non-Arrhenius self-diffusivities characteristic of bcc Ti.

cond-mat.mtrl-sci↗
arXiv2016

Fermi-liquid behavior and thermal conductivity of ε-iron at Earth's core conditions

The electronic state and transport properties of hot dense iron are of the utmost importance to geophysics. Combining the density functional and dynamical mean field theories we study the impact of electron correlations on electrical and thermal resistivity of hexagonal close-packed $ε$-Fe at Earth's core conditions. $ε$-Fe is found to behave as a nearly perfect Fermi liquid. The quadratic dependence of the scattering rate in Fermi liquids leads to a modification of the Wiedemann-Franz law with suppression of the thermal conductivity as compared to the electrical one. This significantly increases the electron-electron thermal resistivity which is found to be of comparable magnitude to the electron-phonon one. The implications of this effect on the dynamics of Earth's core is discussed.

cond-mat.str-el↗
arXiv2015

First-principles study of configurational disorder in B$_{4}$C using a superatom-special quasirandom structure method

Configurationally disordered crystalline boron carbide, B$_{4}$C, is studied using first-principles calculations. We investigate both dilute and high concentrations of carbon-boron substitutional defects. For the latter purpose, we suggest a superatom's picture of the complex structure and combine it with a special quasi-random structure approach for disorder. In this way, we model a random distribution of high concentrations of the identified low-energy defects: 1) Bipolar defects and 2) Rotation of icosahedral carbon among the three polar-up sites. Additionally, the substitutional disorder of the icosahedral carbon at all six polar sites, as previously discussed in the literature, is also considered. Two configurational phase transitions from the ordered to the disordered configurations are predicted to take place upon increasing temperature using a mean-field approximation for the entropy. The first transition, at 870 K, induces substitutional disorder of the icosahedral carbon atoms among the three polar-up sites, meanwhile the second transition, at 2325 K, reveals the random substitution of the icosahedral carbon atoms at all six polar sites coexisting with bipolar defects. Already the first transition removes the monoclinic distortion existing in the ordered ground state configuration and restore the rhombohedral system (R3m). The restoration of inversion symmetry yielding the full rhombohedral symmetry (R-3m) on average, corresponding to what is reported in the literature, is achieved after the second transition. The electronic density of states, obtained from the disordered phases indicates a sensitivity of band gap to the degree of configurational disorder in B$_{4}$C.

cond-mat.mtrl-sci↗
arXiv2015

Configurational order-disorder induced metal-nonmetal transition in B$_{13}$C$_{2}$ studied with first-principles superatom-special quasirandom structure method

Due to a large discrepancy between theory and experiment, the electronic character of crystalline boron carbide B$_{13}$C$_{2}$ has been a controversial topic in the field of icosahedral boron-rich solids. We demonstrate that this discrepancy is removed when configurational disorder is accurately considered in the theoretical calculations. We find that while ordered ground state B$_{13}$C$_{2}$ is metallic, configurationally disordered B$_{13}$C$_{2}$, modeled with a superatom-special quasirandom structure method, goes through a metal to non-metal transition as the degree of disorder is increased with increasing temperature. Specifically, one of the chain-end carbon atoms in the CBC chains substitutes a neighboring equatorial boron atom in a B$_{12}$ icosahedron bonded to it, giving rise to a B$_{11}$C$^{e}$(BBC) unit. The atomic configuration of the substitutionally disordered B$_{13}$C$_{2}$ thus tends to be dominated by a mixture between B$_{12}$(CBC) and B$_{11}$C$^{e}$(BBC). Due to splitting of valence states in B$_{11}$C$^{e}$(BBC), the electron deficiency in B$_{12}$(CBC) is gradually compensated.

cond-mat.mtrl-sci↗
arXiv2014

Electronic correlations in Fe at Earth's inner core conditions: effect of doping with Ni

We have studied the body-centered cubic (bcc), face-centered cubic (fcc) and hexagonal close-packed (hcp) phases of Fe alloyed with 25 at. % of Ni at Earth's core conditions using an ab initio local density approximation + dynamical mean-field theory (LDA+DMFT) approach. The alloys have been modeled by ordered crystal structures based on the bcc, fcc, and hcp unit cells with minimum possible cell size allowing for the proper composition. Our calculations demonstrate that the strength of electronic correlations on the Fe 3d shell is highly sensitive to the phase and local environment. In the bcc phase the 3d electrons at the Fe site with Fe only nearest neighbors remain rather strongly correlated even at extreme pressure-temperature conditions, with the local and uniform magnetic susceptibility exhibiting a Curie-Weiss-like temperature evolution and the quasi-particle lifetime Γ featuring a non-Fermi-liquid temperature dependence. In contrast, for the corresponding Fe site in the hcp phase we predict a weakly-correlated Fermi-liquid state with a temperature-independent local susceptibility and a quadratic temperature dependence of Γ. The iron sites with nickel atoms in the local environment exhibit behavior in the range between those two extreme cases, with the strength of correlations gradually increasing along the hcp-fcc-bcc sequence. Further, the inter-site magnetic interactions in the bcc and hcp phases are also strongly affected by the presence of Ni nearest neighbors. The sensitivity to the local environment is related to modifications of the Fe partial density of states due to mixing with Ni 3d-states.

cond-mat.str-el↗
arXiv2013

Electronic properties and magnetism of iron at the Earth's inner core conditions

We employ state-of-the-art ab initio simulations within the dynamical mean-field theory to study three likely phases of iron (hexogonal close-packed, hcp, face centered cubic, fcc, and body centered cubic, bcc) at the Earth's core conditions. We demonstrate that the correction to the electronic free energy due to correlations can be significant for the relative stability of the phases. The strongest effect is observed in bcc Fe, which shows a non-Fermi liquid behaviour, and where a Curie-Weiss behaviour of the uniform susceptbility hints at a local magnetic moment still existing at 5800 K and 300 GPa. We predict that all three structures have sufficiently high magnetic susceptibility to stabilize the geodynamo.

cond-mat.str-el↗
arXiv2011

Lattice dynamics of anharmonic solids from first principles

An accurate and easily extendable method to deal with lattice dynamics of solids is offered. It is based on first-principles molecular dynamics simulations and provides a consistent way to extract the best possible harmonic - or higher order - potential energy surface at finite temperatures. It is designed to work even for strongly anharmonic systems where the traditional quasiharmonic approximation fails. The accuracy and convergence of the method are controlled in a straightforward way. Excellent agreement of the calculated phonon dispersion relations at finite temperature with experimental results for bcc Li and bcc Zr is demonstrated.

cond-mat.mtrl-sci↗
arXiv2003

Van der Waals Density Functional for Layered Structures

To understand sparse systems we must account for both strong local atom bonds and weak nonlocal van der Waals forces between atoms separated by empty space. A fully nonlocal functional form [H. Rydberg, B.I. Lundqvist, D.C. Langreth, and M. Dion, Phys. Rev. B 62, 6997 (2000)] of density-functional theory (DFT) is applied here to the layered systems graphite, boron nitride, and molybdenum sulfide to compute bond lengths, binding energies, and compressibilities. These key examples show that the DFT with the generalized-gradient approximation does not apply for calculating properties of sparse matter, while use of the fully nonlocal version appears to be one way to proceed.

cond-mat.mtrl-sci↗
arXiv2002

Stability of gold nanowires at large Au-Au separations

The unusual structural stability of gold nanowires at large separations of gold atoms is explained from first-principles quantum mechanical calculations. We show that undetected light atoms, in particular hydrogen, stabilize the experimentally observed structures, which would be unstable in pure gold wires. The enhanced cohesion is due to the partial charge transfer from gold to the light atoms. This finding should resolve a long-standing controversy between theoretical predictions and experimental observations.

cond-mat.mtrl-sci↗
arXiv2002

Screened Coulomb interactions in metallic alloys: II Screening beyond the single-site and atomic sphere approximations

A quantitative description of the configurational part of the total energy of metallic alloys with substantial atomic size difference cannot be achieved in the atomic sphere approximation: It needs to be corrected at least for the multipole moment interactions in the Madelung part of the one-electron potential and energy. In the case of a random alloy such interactions can be accounted for only by lifting the atomic sphere and single-site approximations, in order to include the polarization due to local environment effects. Nevertheless a simple parameterization of the screened Coulomb interactions for the ordinary single-site methods, including the generalized perturbation method, is still possible. We obtained such a parameterization for bulk and surface NiPt alloys, which allows one to obtain quantitatively accurate effective interactions in this system.

cond-mat.mtrl-sci↗