Search results for "DENSITY FUNCTIONAL THEORY"
showing 10 items of 981 documents
Small radius electron and hole polarons in PbX2 (X = F, Cl, Br) crystals: a computational study
2021
First-principles hybrid density functional theory (DFT) calculations were performed for small radius polarons – self-trapped electrons (STELs) and holes (STHs) in PbX2 (X = F, Cl, Br) crystals, widely used as parent materials for inorganic halide perovskites (CsPbX3) and scintillators. The atomic and electronic structures, spin and charge distributions and formation energies for both types of polarons were predicted for orthorhombic PbF2 and STELs for cubic PbF2. The STH structure was identified in a controversial case of PbCl2. We also confirmed and analyzed in detail experimentally suggested configurations for other cases. It is shown how, due to a delicate balance of ionic and covalent c…
Two-dimensional hydrogenated buckled gallium arsenide: an ab initio study
2020
First-principles calculations have been carried out to investigate the stability, structural and electronic properties of two-dimensional (2D) hydrogenated GaAs with three possible geometries: chair, zigzag-line and boat configurations. The effect of van der Waals interactions on 2D H-GaAs systems has also been studied. These configurations were found to be energetic and dynamic stable, as well as having a semiconducting character. Although 2D GaAs adsorbed with H tends to form a zigzag-line configuration, the energy differences between chair, zigzag-line and boat are very small which implies the metastability of the system. Chair and boat configurations display a [Formula: see text]-[Formu…
Density functional study of gold atoms and clusters on a graphite (0001) surface with defects
2006
Adsorption of gold atoms and clusters $(N=6)$ on a graphite (0001) surface with defects has been studied using density functional theory. In addition to perfect graphite (0001), three types of surface defects have been considered: a surface vacancy (hole), a pyridinelike defect comprising three grouped nitrogen atoms, and a substitutional doping by N or B. Results for Au and ${\mathrm{Au}}_{6}$ indicate that the surface vacancy can form chemical bonds with Au as the three nearby carbons align their dangling bonds towards the gold particle (binding energy 2.4--$2.6\phantom{\rule{0.3em}{0ex}}\mathrm{eV}$). A similar chemically saturated holelike construction with three pyridinic N atoms resul…
First-principles modeling of oxygen interaction with SrTiO3(001) surface: Comparative density-functional LCAO and plane-wave study
2011
Large scale first-principles calculations based on density functional theory (DFT) employing two different methods (atomic orbitals and plane wave basis sets) were used to study the energetics, geometry, the electronic charge redistribution and migration for adsorbed atomic and molecular oxygen on defect-free SrTiO3(001) surfaces (both SrO- and TiO2-terminated), which serves as a prototype for many ABO3-type perovskites. Both methods predict substantial binding energies for atomic O adsorption at the bridge position between the oxygen surface ions and an adjacent metal ion. A strong chemisorption is caused by formation of a surface molecular peroxide ion. In contrast, the neutral molecular …
A comparative study of Ag and Cu adhesion on an MgO(001) surface
2004
Abstract Ab initio calculations were performed on 2D slab models of copper and silver adhesion on a perfect MgO(001) surface using density functional theory (DFT) combined with the localized atomic wave functions, as implemented in both CRYSTAL-98 and CRYSTAL-03 computer codes. To clarify the nature of the interfacial bonding, we consider slab models of the Ag/MgO(001) and Cu/MgO(001) interfaces with six different substrate coverages, varied from 1 4 monolayer (ML) up to 2 ML. The dependence of several key interface properties on the substrate coverage is analyzed. For all coverages, the most favorable sites for the adsorption of metal atoms are found to be above the surface O 2− ions, wher…
Impact of anionic system modification on the desired properties for CuGa(S1−Se )2 solid solutions
2021
Abstract One of promising directions of the modern solar cells’ development is related to the use of the ternary chalcopyrite crystals (CuInS2, CuGaS2 etc.) and their solid solutions as efficient light absorbing layers. Unfortunately, so far there is no systematic research linking chemical composition to useful properties allowing their optimization to increase the efficiency of solar cells. Therefore, we report the results of the detailed theoretical studies of the structural, electronic, and optical properties for the series of CuGa(S1−xSex)2 solid solutions (x = 0, 0.25, 0.5, 0.75, 1) in the framework of the density functional theory. For this purpose, crystal structures are analyzed wit…
Structural and Mössbauer study of (Sb0.70Te0.30)100-x Snx alloys with x = 0, 2.5, 5.0 and 7.5
2019
(Sb 0.70 Te 0.30 ) 100-x Sn x alloys (with x = 0, 2.5, 5.0 and 7.5 at. %)have been synthesized and characterized in order to determine the crystalline structure and properties of materials obtained upon solidification and to extract information about the location of the Sn atom in the Sb-Te matrix. Powder X-ray diffraction (XRD)has been used to determine the crystalline structure, whereas Mössbauer spectroscopy has been utilized to determine the localization and the local structure of the Sn atom in the Sb-Te matrix through the hyperfine interactions of the 119 Sn probe with its environment. We found that Sb 70 Te 30 crystallizes in a trigonal structure belonging to P-3m1 space group, while…
Revealing Charge-Transfer Dynamics at Electrified Sulfur Cathodes Using Constrained Density Functional Theory
2021
To understand and control the behavior of electrochemical systems, including batteries and electrocatalysts, we seek molecular-level details of the charge transfer mechanisms at electrified interfaces. Recognizing some key limitations of standard equilibrium electronic structure methods to model materials and their interfaces, we propose applying charge constraints to effectively separate electronic and nuclear degrees of freedom, which are especially beneficial to the study of conversion electrodes, where electronic charge carriers are converted to much slower polarons within a material that is nonmetallic. We demonstrate the need for such an approach within the context of sulfur cathodes …
Nitrogen Hydrate Cage Occupancy and Bulk Modulus Inferred from Density Functional Theory-Derived Cell Parameters
2021
International audience; Gas clathrate hydrate solid materials, ubiquitous in nature as found either on the ocean floor, permafrost on the Earth, or in extraterrestrial planets and comets, are also technologically relevant, for example, in energy storage or carbon dioxide sequestration. Nitrogen hydrate, in particular, is of great interest as a promoter of the kinetics of the methane replacement reaction by carbon dioxide in natural gas hydrates. This hydrate may also appear in the chemistry of planets wherever nitrogen constitutes the majority of the atmosphere. A fine understanding of the stability of this hydrate under various thermodynamic conditions is thus of utmost importance to asses…
Electronic structure calculations with GPAW: a real-space implementation of the projector augmented-wave method.
2011
Electronic structure calculations have become an indispensable tool in many areas of materials science and quantum chemistry. Even though the Kohn-Sham formulation of the density-functional theory (DFT) simplifies the many-body problem significantly, one is still confronted with several numerical challenges. In this article we present the projector augmented-wave (PAW) method as implemented in the GPAW program package (https://wiki.fysik.dtu.dk/gpaw) using a uniform real-space grid representation of the electronic wavefunctions. Compared to more traditional plane wave or localized basis set approaches, real-space grids offer several advantages, most notably good computational scalability an…