arXiv subjects

Peter Blaha

Publications and source records attributed to Peter Blaha.

41 records · Page 3Linked to original sources

arXiv2011

Implementation of screened hybrid functionals based on the Yukawa potential within the LAPW basis set

The implementation of screened hybrid functionals into the WIEN2k code, which is based on the LAPW basis set, is reported. The Hartree-Fock exchange energy and potential are screened by means of the Yukawa potential as proposed by Bylander and Kleinman [Phys. Rev. B 41, 7868 (1990)] for the calculation of the electronic structure of solids with the screened-exchange local density approximation. Details of the formalism, which is based on the method of Massidda, Posternak, and Baldereschi [Phys. Rev. B 48, 5058 (1993)] for the unscreened Hartree-Fock exchange are given. The results for the transition-energy and structural properties of several test cases are presented. Results of calculations of the Cu electric-field gradient in Cu2O are also presented, and it is shown that the hybrid functionals are much more accurate than the standard local-density or generalized gradient approximations.

cond-mat.mtrl-sci↗

arXiv2011

Spin-state crossover and hyperfine interactions of ferric iron in MgSiO$_3$ perovskite

Using density functional theory plus Hubbard $U$ calculations, we show that the ground state of (Mg,Fe)(Si,Fe)O$_3$ perovskite, a major mineral phase in the Earth's lower mantle, has high-spin ferric iron ($S=5/2$) at both the dodecahedral (A) and octahedral (B) site. As the pressure increases, the B-site iron undergoes a spin-state crossover to the low-spin state ($S=1/2$), while the A-site iron remains in the high-spin state. Our calculation shows that the B-site spin-state crossover in the pressure range of 40-70 GPa is accompanied by a noticeable volume reduction and an increase in quadrupole splitting, consistent with recent X-ray diffraction and Mössbauer spectroscopy measurements. The volume reduction leads to a significant softening in the bulk modulus, which suggests a possible source of seismic velocity anomalies in the lower mantle.

physics.geo-ph↗

arXiv2010

Systematic investigation of a family of gradient-dependent functionals for solids

Eleven density functionals are compared with regard to their performance for the lattice constants of solids. We consider standard functionals, such as the local-density approximation and the Perdew-Burke-Ernzerhof (PBE) generalized-gradient approximation (GGA), as well as variations of PBE GGA, such as PBEsol and similar functionals, PBE-type functionals employing a tighter Lieb-Oxford bound, and combinations thereof. Several of these variations are proposed here for the first time. On a test set of 60 solids we perform a system-by-system analysis for selected functionals and a full statistical analysis for all of them. The impact of restoring the gradient expansion and of tightening the Lieb-Oxford bound is discussed, and confronted with previous results obtained from other codes, functionals or test sets. No functional is uniformly good for all investigated systems, but surprisingly, and pleasingly, the simplest possible modifications to PBE turn out to have the most beneficial effect on its performance. The atomization energy of molecules was also considered and on a testing set of six molecules, we found that the PBE functional is clearly the best, the others leading to strong overbinding.

cond-mat.mtrl-sci↗

arXiv2009

The Small Unit Cell Reconstructions of SrTiO3 (111)

We analyze the basic structural units of simple reconstructions of the (111) surface of SrTiO3 using density functional calculations. The prime focus is to answer three questions: what is the most appropriate functional to use; how accurate are the energies; what are the dominant low-energy structures and where do they lie on the surface phase diagram. Using test calculations of representative small molecules we compare conventional GGA with higher-order methods such as the TPSS meta-GGA and on-site hybrid methods PBE0 and TPSSh, the later being the most accurate. There are large effects due to reduction of the metal d oxygen sp hybridization when using the hybrid methods which are equivalent to a dynamical GGA+U, which leads to rather substantial improvements in the atomization energies of simple calibration molecules, even though the d-electron density for titanium compounds is rather small. By comparing the errors of the different methods we are able to generate an estimate of the theoretical error, which is about 0.25eV per 1x1 unit cell, with changes of 0.5-1.0 eV per 1x1 cell with the more accurate method relative to conventional GGA. An analysis of the plausible structures reveals an unusual low-energy TiO2-rich configuration with an unexpected distorted trigonal biprismatic structure. This structure can act as a template for layers of either TiO or Ti2O3, consistent with experimental results as well as, in principle, Magnelli phases. The results also suggest that both the fracture surface and the stoichiometric SrTiO3 (111) surface should spontaneously disproportionate into SrO and TiO2 rich domains, and show that there are still surprises to be found for polar oxide surfaces.

cond-mat.mtrl-sci↗

arXiv1999

Improving the Efficiency of FP-LAPW Calculations

The full-potential linearized augmented-plane wave (FP-LAPW) method is well known to enable most accurate calculations of the electronic structure and magnetic properties of crystals and surfaces. The implementation of atomic forces has greatly increased it's applicability, but it is still generally believed that FP-LAPW calculations require substantial higher computational effort compared to the pseudopotential plane wave (PPW) based methods. In the present paper we analyse the FP-LAPW method from a computational point of view. Starting from an existing implementation (WIEN95 code), we identified the time consuming parts and show how some of them can be formulated more efficiently. In this context also the hardware architecture plays a crucial role. The remaining computational effort is mainly determined by the setup and diagonalization of the Hamiltonian matrix. For the latter, two different iterative schemes are compared. The speed-up gained by these optimizations is compared to the runtime of the ``original'' version of the code, and the PPW approach. We expect that the strategies described here, can also be used to speed up other computer codes, where similar tasks must be performed.

cond-mat↗