Self-consistent tight-binding atomic-relaxation model of titanium dioxide

Schelling, Patrick K.; Yu, Naichang; Halleý, J. W.

doi:10.1103/physrevb.58.1279

Cited by 75 publications

(44 citation statements)

References 26 publications

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“…The partial covalent character of zirconia has already been postulated 22 and is evident from electronic structure calculations based on density functional theory. In this paper we further investigate the recently proposed polarizable self-consistent tight binding (SC-TB) model [23][24][25] which combines the physical concepts of covalency, ionicity and polarizability. Using the SC-TB model we are drawn to the conclusion that the covalent character of the Zr-O bond makes a significant contribution to the relative energetics of different structures, which would explain the limited predictive power of the previous ionic models.…”

Section: Introductionmentioning

confidence: 99%

Relative energetics and structural properties of zirconia using a self-consistent tight-binding model

2000

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We describe an empirical, self-consistent, orthogonal tight-binding model for zirconia, which allows for the polarizability of the anions at dipole and quadrupole levels and for crystal field splitting of the cation d orbitals. This is achieved by mixing the orbitals of different symmetry on a site with coupling coefficients driven by the Coulomb potentials up to octapole level. The additional forces on atoms due to the self-consistency and polarizabilities are exactly obtained by straightforward electrostatics, by analogy with the Hellmann-Feynman theorem as applied in first-principles calculations. The model correctly orders the zero temperature energies of all zirconia polymorphs. The Zr-O matrix elements of the Hamiltonian, which measure covalency, make a greater contribution than the polarizability to the energy differences between phases. Results for elastic constants of the cubic and tetragonal phases and phonon frequencies of the cubic phase are also presented and compared with some experimental data and first-principles calculations. We suggest that the model will be useful for studying finite temperature effects by means of molecular dynamics. 31.15. Ar,71.15.Fv,

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Section: Introductionmentioning

confidence: 99%

Relative energetics and structural properties of zirconia using a self-consistent tight-binding model

2000

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“…The results give excellent values for the work functions of low index rutile surfaces and very reasonable numbers for the surface energies and surface relaxation of low index surfaces 7 . The molecular dynamics version of this code was used to study the structure of polarons in rutile as a function of temperature for the first time 8 .…”

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confidence: 82%

Final Report for Department of Energy grant DE-FG02-91ER45455, "Theoretical Study of Reactions at the Electrode-Electrolyte Interface"

Halleý¹

2009

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In this project, reaction rates were predicted by numerical methods, in a collaboration with Argonne National Laboratory . Emphasis is on electron transfer and transport involving ions known to be important in enhancing stress corrosion cracking in light water reactors and on electron transfer at oxide surfaces. In the latter part of the grant period we placed increased emphasis on development and use of self consistent tight binding methods for this kind of study. We showed that by careful fitting of results from first principles plane wave calculations,we could model surfaces and interfaces oxides and metals using these methods. We obtained results for the titanium/titanium oxide interface in this way and completed a model of the ruthenium dioxide surface using our innovative self consistent tight binding molecular dynamics methods. We completed development of a description of liquid water within the self consistent tight binding context and studied the rutile water 110 interface to determine if it is hydroxylated. A self consistent tight binding study of titanium metal surfaces demonstrated the usefulness of this method for metals. In collaboration with the Argonne group, we extended the tight binding calculations on rutile titania to the anatase form and made the first calculations of the relative stability of anatase and rutile as a function of crystallite size. We completed studies of small anatase particles in water using the method and found significant distortions of nanoparticle crystallite shapes as a consequence of interactions with the water.

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“…For these reasons, we have been modeling the surface of Pt and its interactions with H and O using a self consistent semi-empirical electronic structure method called self consistent tight binding (SCTB) [10][11][12][13][14][15][16][17][18][19][20] which permits direct dynamics study of larger systems than can be accessed with full first principles methods. In this paper we describe our method of extending the SCTB method to take account of relativistic effects on the level of the spin-orbit interaction 21 (SO-SCTB).…”

Section: Pacs Numbersmentioning

confidence: 99%

“…As in the self consistent tight binding (SCTB) method which we developed previously [10][11][12][13][14][15][16][17][18][19][20] the direct dynamics problem is described by the following energy functional (see 10 for the origin of this functional) …”

Section: Relativistic Sctbmentioning

confidence: 99%

Relativistic tight-binding model: Application to Pt surfaces

Tchernatinsky

Halleý

2011

Phys. Rev. B

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We report a parametrization of a previous self consistent tight binding model, suitable for metals with high atomic number in which nonscalar relativistic effects are significant in the electron physics of condensed phases. The method is applied to platinum. The model is fitted to DFT band structures and cohesive energies and spectroscopic data on platinum atoms in 5 oxidation states and is then shown without further parametrization to correctly reproduce several low index surface structures. We also predict reconstructions of some vicinal surfaces.

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Self-consistent tight-binding atomic-relaxation model of titanium dioxide

Cited by 75 publications

References 26 publications

Relative energetics and structural properties of zirconia using a self-consistent tight-binding model

Relative energetics and structural properties of zirconia using a self-consistent tight-binding model

Final Report for Department of Energy grant DE-FG02-91ER45455, "Theoretical Study of Reactions at the Electrode-Electrolyte Interface"

Relativistic tight-binding model: Application to Pt surfaces

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