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Journal ArticleDOI

From ultrasoft pseudopotentials to the projector augmented-wave method

15 Jan 1999-Physical Review B (American Physical Society)-Vol. 59, Iss: 3, pp 1758-1775
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
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Journal ArticleDOI
22 Jun 2012-Science
TL;DR: Ab initio molecular dynamics simulations reveal the phase-change kinetics in PCRAM devices and the structural origin of the incubation-assisted increase in crystallization speed, which paves the way for achieving a broadly applicable memory device, capable of nonvolatile operations beyond gigahertz data-transfer rates.
Abstract: Phase-change random-access memory (PCRAM) is one of the leading candidates for next-generation data-storage devices, but the trade-off between crystallization (writing) speed and amorphous-phase stability (data retention) presents a key challenge. We control the crystallization kinetics of a phase-change material by applying a constant low voltage via prestructural ordering (incubation) effects. A crystallization speed of 500 picoseconds was achieved, as well as high-speed reversible switching using 500-picosecond pulses. Ab initio molecular dynamics simulations reveal the phase-change kinetics in PCRAM devices and the structural origin of the incubation-assisted increase in crystallization speed. This paves the way for achieving a broadly applicable memory device, capable of nonvolatile operations beyond gigahertz data-transfer rates.

690 citations

Journal ArticleDOI
TL;DR: A generalized solid-state nudged elastic band (G-SSNEB) method is presented for determining reaction pathways of solid-solid transformations involving both atomic and unit-cell degrees of freedom and it is demonstrated that the method is robust for mechanisms dominated either by atomic motion or by unit- cell deformation.
Abstract: A generalized solid-state nudged elastic band (G-SSNEB) method is presented for determining reaction pathways of solid–solid transformations involving both atomic and unit-cell degrees of freedom. We combine atomic and cell degrees of freedom into a unified description of the crystal structure so that calculated reaction paths are insensitive to the choice of periodic cell. For the rock-salt to wurtzite transition in CdSe, we demonstrate that the method is robust for mechanisms dominated either by atomic motion or by unit-cell deformation; notably, the lowest-energy transition mechanism found by our G-SSNEB changes with cell size from a concerted transformation of the cell coordinates in small cells to a nucleation event in large cells. The method is efficient and can be applied to systems in which the force and stress tensor are calculated using density functional theory.

687 citations

Journal ArticleDOI
TL;DR: Experimental measurements and density functional theory calculations indicate that the formation of the Fe═O intermediate structure is a key step to promoting the conversion of benzene to phenol, paving the way toward highly efficient nonprecious catalysts for low-temperature oxidation reactions in heterogeneous catalysis and electrocatalysis.
Abstract: Coordinatively unsaturated (CUS) iron sites are highly active in catalytic oxidation reactions; however, maintaining the CUS structure of iron during heterogeneous catalytic reactions is a great challenge. Here, we report a strategy to stabilize single-atom CUS iron sites by embedding highly dispersed FeN4 centers in the graphene matrix. The atomic structure of FeN4 centers in graphene was revealed for the first time by combining high-resolution transmission electron microscopy/high-angle annular dark-field scanning transmission electron microscopy with low-temperature scanning tunneling microscopy. These confined single-atom iron sites exhibit high performance in the direct catalytic oxidation of benzene to phenol at room temperature, with a conversion of 23.4% and a yield of 18.7%, and can even proceed efficiently at 0°C with a phenol yield of 8.3% after 24 hours. Both experimental measurements and density functional theory calculations indicate that the formation of the Fe═O intermediate structure is a key step to promoting the conversion of benzene to phenol. These findings could pave the way toward highly efficient nonprecious catalysts for low-temperature oxidation reactions in heterogeneous catalysis and electrocatalysis.

678 citations

Journal ArticleDOI
TL;DR: In this paper, a crystalline tri-s-triazine-based graphitic carbon nitride (g-CN) was synthesized for hydrogen and oxygen production from water splitting.
Abstract: Graphitic carbon nitride (g-CN) is an emerging metal-free photocatalyst for solar energy conversion via water splitting and CO2 fixation. Herein, we used preheated melamine as a starting material in combination with the salt melt method to synthesize a crystalline tri-s-triazine-based g-CN. The as-obtained sample exhibited high stability and photocatalytic activity toward hydrogen and oxygen production from water splitting. In addition, by adding phosphate to mimic natural photosynthetic environment, the apparent quantum yield (AQY) for the hydrogen production reached 50.7% at 405 nm, which is the highest value ever reported for conjugated carbon nitride polymers in hydrogen evolution photocatalysis. The results of this study demonstrate that crystalline covalent tri-s-triazine frameworks hold great promise for solar energy applications.

677 citations

Journal ArticleDOI
TL;DR: In this paper, the geometry and electronic structure of reduced ceria surfaces with oxygen vacancies were examined using first principles density functional theory (DFT), with the inclusion of on site electronic correlations, and it was shown that the (1, 1, 0) surface has the lowest vacancy formation energy.

670 citations

References
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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