Ab initio calculations of phonon transport in ZnO and ZnS

We present an approach to calculate ballistic phonon transport that combines the atomistic Green’s function (AGF) method with ab initio results. For the interatomic potential we use the harmonic approach. The equilibrium positions of the atoms and the interatomic force constants (ifcs) are calculated using the ABINIT program package [X. Gonze et al., Z. Kristallogr. 220, 558 (2005)], which is based on density functional theory. Therefore, the presented approach is parameter free. From the Green’s function of the system we determine the density of states as well as the transmission function. The thermal conductance is obtained within the linear response regime. We apply this approach to bulk ZnO and bulk ZnS. Transmission functions for different transport directions for each material are presented. A comparison of the transmission function shows, that a ZnO/ZnS interface could be a promising phonon blocker. Adding such interfaces in ZnO or ZnS based thermoelectric devices could therefore increase the figure of merit.     

The non-pair forces and phonon dispersion in heavy alkali metals

Two types of the non-pair forces, one from the Born-Mayer and other from the Morse potential, are derived to discuss the response of the electrons in heavy alkali metals, i.e. rubidium and caesium. These potentials are added to the two-body potential of Morse to account for the ion-ion interactions as well. The potentials so obtained are employed to predict the phonon dispersion relations in the bcc metals, which are also compared with the recent precise neutron scattering data.     

Ab initio investigations of phonon anomalies and superconductivity in the rock-salt YS

The phonon spectrum, phonon linewidths and electron–phonon coupling parameter for YS have been calculated by using a first-principles scheme, based on the application of the plane-wave pseudopotential method, density functional theory, and a linear response technique. Our phonon results confirm the presence of anomalous features in the neutron-scattering spectrum for the longitudinal acoustic branch. It is shown that the electronic d-state effects are primarily responsible for the anomalous phonon behaviour. The calculated values of phonon linewidths along various symmetry directions are presented and discussed. The longitudinal acoustic phonon linewidth shows a maximum at the zone boundary L where the branch exhibits a pronounced dip. The calculated electron–phonon coupling parameter,?λ?= 0.52, compares very well with a previous empirical value of 0.56.     

Ab initio investigation of phonon spectra in GdLiF4 compound under hydrostatic pressure

Employing density functional theory (DFT) within the generalized gradient approximation, the GdLiF₄ structure has been studied for a pressure range from 0 to 12 GPa. The influence of pressure on the lattice vibrational spectrum of the scheelite phase (I4₁/a, Z = 4) has been evaluated by means the “direct” approach, i.e., using force constants calculated from atomic displacements. As a result the Raman and infrared modes have been identified and their dependencies on pressure have been investigated and compared with available experimental data. It has been found that instability of the crystal structure appears at pressures above 6 GPa.     

Ab initio phonon dispersion relations of $\mathsf{\alpha}$-Ga

We present the ab initio phonon dispersion relations of -Ga. The calculations are carried out within density functional perturbation theory by using either norm-conserving pseudopotential and 4s and 4p electrons in the valence or ultrasoft pseudopotential and 3d electrons in the valence as well. The inclusion of 3d electrons in the valence turned out to be necessary to better reproduce the experimental frequencies of the stretching modes of the Ga₂ dimers present in the -Ga structure.Received: 29 July 2003, Published online: 19 November 2003PACS: 63.20.Dj Phonon states and bands, normal modes, and phonon dispersion - 71.15.Nc Total energy and cohesive energy calculations - 71.15.Mb Density functional theory, local density approximation, gradient and other corrections     

Ab initio many-body treatment of the electronic structure of metals

We propose and apply a combination of an ab initio (band-structure) calculation with a many-body treatment including screening effects. We start from a linearized muffin-tin orbital (LMTO) calculation to determine the Bloch functions for the Hartree one-particle Hamiltonian, from which we calculate the static susceptibility and dielectric function within the standard random phase approximation (RPA). From the Bloch functions we obtain maximally localized Wannier functions, using a method proposed by Marzari and Vanderbilt. Within this Wannier basis all relevant one-particle and unscreened and screened Coulomb matrix elements are calculated. This yields a multi-band Hamiltonian in second quantization with ab initio parameters, for which screening has been taken into account within the simplest standard approximation. Then, established methods of many-body theory are used. We apply this concept to a simple metal, namely lithium (Li). Here the maximally localized Wannier functions turn out to be of the sp³-orbital kind. Furthermore, only the on-site contributions of the screened Coulomb matrix elements are relevant, and a generalized, four-band Hubbard model is justified. The screened on-site Coulomb matrix elements are considerably smaller than the band width because of which it is sufficient to calculate the selfenergy in weak-coupling approximation. We compare results obtained within the screened Hartree-Fock approximation (HFA) and within the second-order perturbation theory (SOPT) in the Coulomb matrix elements for Li and find that many-body effects are small but not negligible even for this simple metal.     

Ab initio study of phonon dispersion and thermodynamic properties of pure and doped pyrites

Pyrites (FeS₂) are solid minerals that are found abundantly in Nigeria and are easy to prepare in laboratories. In this work, FeS₂ is studied extensively in its pure state as well as when iron is substitutionally doped with zinc and calcium at concentrations of 0, 0.25, 0.5, 0.75 and 1. Using density functional theory, the eectronic, dynamic and thermodynamic properties were calculated. The results revealed that the lattice parameters and bulk modulus increases with increasing concentration and the obtained values are in agreement with available experimental and theoretical values. Though pyrite, when doped with zinc, obeys Vegard’s law, doping with calcium revealed pronounced deviation from this law. The calculated band structures showed that FeS₂ has an indirect band gap whose size decreases after introducing zinc while doping with calcium increases the band gap. The phonon dispersion of the end members FeS₂ and ZnS₂ indicate that the systems are dynamically stable while CaS₂ is dynamically unstate. Also, the thermodynamic properties of the pure and doped pyrites were calculated and the ranges of temperature at which the lattice and electronic degrees of freedom contribute to the specific heat capacity are presented.     

Ab initio calculations of generalized-stacking-fault energy surfaces and surface energies for FCC metals

The ab initio calculations have been used to study the generalized-stacking-fault energy (GSFE) surfaces and surface energies for the closed-packed (1 1 1) plane in FCC metals Cu, Ag, Au, Ni, Al, Rh, Ir, Pd, Pt, and Pb. The GSFE curves along (1 1 1) direction and (1 1 1) direction, and surface energies have been calculated from first principles. Based on the translational symmetry of the GSFE surfaces, the fitted expressions have been obtained from the Fourier series. Our results of the GSFEs and surface energies agree better with experimental results. The metals Al, Pd, and Pt have low γ_us/γ_I value, so full dislocation will be observed easily; while Cu, Ag, Au, and Ni have large γ_us/γ_I value, so it is preferred to create partial dislocation. From the calculations of surface energies, it is confirmed that the VIII column elements Ni, Rh, Ir, Pd, and Pt have higher surface energies than other metals.     

Ab initio calculations of thermal conductivity of metals with hot electrons

Warm dense matter (WDM) is a state of a substance with a solid-state density and temperature from 1 to 100 eV. Researchers believe that such a state exists in the cores of giant planets. Investigation of WDM is important for some applications, such as surface treatment on the nanometer scale, laser ablation, and the formation of the plasma sources of the X-ray radiation into the inertial synthesis. In this study, the conductivity and the thermal conductivity are calculated based on density functional theory and the Kubo-Greenwood theory. This approach was already used to simulate the transport properties in a broad range of densities and temperatures, and its efficiency has been demonstrated. The conductivity and the thermal conductivity of aluminum and gold are investigated. Both the isothermal state, when the electron temperature equals the ion temperature, and the two-temperature state, when the electron temperature exceeds the ion temperature, are considered. The calculations were performed for a solid body and liquid in the range of electron temperatures from 0 to 6 eV.