From ultrasoft pseudopotentials to the projector augmented-wave method
TL;DR: In this paper, the formal relationship between US Vanderbilt-type pseudopotentials and Blochl's projector augmented wave (PAW) method is derived and the Hamilton operator, the forces, and the stress tensor are derived for this modified PAW functional.
Abstract: The formal relationship between ultrasoft (US) Vanderbilt-type pseudopotentials and Bl\"ochl's projector augmented wave (PAW) method is derived. It is shown that the total energy functional for US pseudopotentials can be obtained by linearization of two terms in a slightly modified PAW total energy functional. The Hamilton operator, the forces, and the stress tensor are derived for this modified PAW functional. A simple way to implement the PAW method in existing plane-wave codes supporting US pseudopotentials is pointed out. In addition, critical tests are presented to compare the accuracy and efficiency of the PAW and the US pseudopotential method with relaxed core all electron methods. These tests include small molecules $({\mathrm{H}}_{2}{,\mathrm{}\mathrm{H}}_{2}{\mathrm{O},\mathrm{}\mathrm{Li}}_{2}{,\mathrm{}\mathrm{N}}_{2}{,\mathrm{}\mathrm{F}}_{2}{,\mathrm{}\mathrm{BF}}_{3}{,\mathrm{}\mathrm{SiF}}_{4})$ and several bulk systems (diamond, Si, V, Li, Ca, ${\mathrm{CaF}}_{2},$ Fe, Co, Ni). Particular attention is paid to the bulk properties and magnetic energies of Fe, Co, and Ni.
Citations
More filters
TL;DR: In this article, the authors used hybrid functionals combined with both plane wave and localized basis sets for a systematic study of the structural and electronic properties of all phases of WO3, and found that hybrid functions work at least as well as the standard DFT/GGA functional in predicting lattice constants and equilibrium volumes.
Abstract: Various hybrid functionals combined with both plane wave and localized basis sets have been used for a systematic study of the structural and electronic properties of all phases of WO3. It is found that hybrid functionals work at least as well as the standard DFT/GGA functional in predicting lattice constants and equilibrium volumes. However, the adoption of hybrid functionals has the advantage to considerably improve the Kohn−Sham band gap which is always severely underestimated by the standard DFT calculations. The HSE06 functional in combination with a plane wave basis set describes well the band gap of WO3, while the B3LYP functional associated with a localized basis set slightly overestimates it. The band gap can be made fully consistent with experiment by fixing the amount of Hartree−Fock exchange in the hybrid functional to 15%.
237 citations
TL;DR: In this paper, the Bethe-Salpeter equation was solved with $G\phantom{\rule{0}{0ex}}W$ wave functions in order to determine the sign and amplitude of the splitting between bright and dark exciton states in the entire Mo{X}_{2}$ and W${X}$ monolayer family.
Abstract: The optical properties of 2D semiconductors made of transition metal dichalcogenide monolayers, such as Mo${X}_{2}$ and W${X}_{2}$ ($X$=S, Se), are dominated by excitons. The light emission yield for optoelectronics applications depends on whether the electron-hole transitions are optically allowed (bright) or forbidden (dark). No direct evidence of the energetic ordering of these exciton states is currently available. The authors here solve the Bethe-Salpeter equation with $G\phantom{\rule{0}{0ex}}W$ wave functions in order to determine the sign and amplitude of the splitting between bright and dark exciton states in the entire Mo${X}_{2}$ and W${X}_{2}$ monolayer family. They also evaluate the influence of pin-orbit coupling on the optical spectra and clearly demonstrate the strong impact of the intravalley Coulomb exchange term on the dark-bright exciton splitting, an important ingredient for engineering optoelectronics and spintronics applications.
237 citations
TL;DR: This work designed a novel two-dimensional (2D) inorganic material, namely Be2 C monolayer, by comprehensive density functional theory (DFT) computations, and it has good stability and is the lowest-energy structure in 2D space confirmed by a global minima search based on the particle-swarm optimization (PSO) method.
Abstract: The design of new materials is an important subject in order to attain new properties and applications, and it is of particular interest when some peculiar topological properties such as reduced dimensionality and rule-breaking chemical bonding are involved. In this work, we designed a novel two-dimensional (2D) inorganic material, namely Be2C monolayer, by comprehensive density functional theory (DFT) computations. In Be2C monolayer, each carbon atom binds to six Be atoms in an almost planar fashion, forming a quasi-planar hexacoordinate carbon (phC) moiety. Be2C monolayer has good stability and is the lowest-energy structure in 2D space confirmed by a global minima search based on the particle-swarm optimization (PSO) method. As a semiconductor with a direct medium band gap, Be2C monolayer is promising for applications in electronics and optoelectronics.
237 citations
TL;DR: Control of biaxial strain in two-dimensional materials based on the growth substrate, enabling more complex low-dimensional electronics, and a dramatic modulation of the band structure.
Abstract: The application of strain to semiconductors allows for controlled modification of their band structure. This principle is employed for the manufacturing of devices ranging from high-performance transistors to solid-state lasers. Traditionally, strain is typically achieved via growth on lattice-mismatched substrates. For two-dimensional (2D) semiconductors, this is not feasible as they typically do not interact epitaxially with the substrate. Here, we demonstrate controlled strain engineering of 2D semiconductors during synthesis by utilizing the thermal coefficient of expansion mismatch between the substrate and semiconductor. Using WSe2 as a model system, we demonstrate stable built-in strains ranging from 1% tensile to 0.2% compressive on substrates with different thermal coefficient of expansion. Consequently, we observe a dramatic modulation of the band structure, manifested by a strain-driven indirect-to-direct bandgap transition and brightening of the dark exciton in bilayer and monolayer WSe2, respectively. The growth method developed here should enable flexibility in design of more sophisticated devices based on 2D materials. Strain engineering is an essential tool for modifying local electronic properties in silicon-based electronics. Here, Ahn et al. demonstrate control of biaxial strain in two-dimensional materials based on the growth substrate, enabling more complex low-dimensional electronics.
236 citations
TL;DR: Two new hydrogen storage reactions are predicted that are some of the most attractive among the presently known ones and combine high gravimetric densities with low enthalpies and are thermodynamically reversible at low pressures due to low vibrational entropies of the product phases containing the [B(12)H(12)](2-) anion.
Abstract: Introduction of economically viable hydrogen cars is hindered by the need to store large amounts of hydrogen. Metal borohydrides [LiBH(4), Mg(BH(4))(2), Ca(BH(4))(2)] are attractive candidates for onboard storage because they contain high densities of hydrogen by weight and by volume. Using a set of recently developed theoretical first-principles methods, we predict currently unknown crystal structures and hydrogen storage reactions in the Li-Mg-Ca-B-H system. Hydrogen release from LiBH(4) and Mg(BH(4))(2) is predicted to proceed via intermediate Li(2)B(12)H(12) and MgB(12)H(12) phases, while for Ca borohydride two competing reaction pathways (into CaB(6) and CaH(2), and into CaB(12)H(12) and CaH(2)) are found to have nearly equal free energies. We predict two new hydrogen storage reactions that are some of the most attractive among the presently known ones. They combine high gravimetric densities (8.4 and 7.7 wt % H(2)) with low enthalpies [approximately 25 kJ/(mol H(2))] and are thermodynamically reversible at low pressures due to low vibrational entropies of the product phases containing the [B(12)H(12)](2-) anion.
236 citations
References
More filters
Book•
31 Dec 1993
TL;DR: The linearized augmented planewave (LAPW) method has emerged as the standard by which density functional calculations for transition metal and rare-earth containing materials are judged.
Abstract: With its extreme accuracy and reasonable computational efficiency, the linearized augmented planewave (LAPW) method has emerged as the standard by which density functional calculations for transition metal and rare-earth containing materials are judged. This volume presents a thorough and self-conta
1,150 citations