We have performed ab initio calculations on a wide range of small molecules, demonstrating the accuracy and flexibility of an alternative method for calculating the electronic structure of molecules, solids, and surfaces. It is based on the local-density approximation (LDA) for exchange and correlation and the nonlinear augmented-plane-wave method. Very accurate atomic forces are obtained directly. This allows for implementation of Car-Parrinello-like techniques to determine simultaneously the self-consistent electron wave functions and the equilibrium atomic positions within an iterative scheme. We find excellent agreement with the best existing LDA-based calculations and remarkable agreement with experiment for the equilibrium geometries, vibrational frequencies, and dipole moments of a wide variety of molecules, including strongly bound homopolar and polar molecules, hydrogen-bound and electron-deficient molecules, and weakly bound alkali and noble-metal dimers, although binding energies are overestimated.
We have investigated the efficacy of ab initio effective potentials in replacing the core electrons of atoms for use in molecular calculations. The effective potentials are obta...
We show than an ab initio molecular-dynamics scheme based on Vanderbilt ultrasoft pseudopotentials and a plane-wave expansion for the electronic orbitals allows one to perform a...
A method is described for obtaining l-dependent relativistic effective core potentials (ECPs) from Dirac–Fock self-consistent field atomic wave functions. These potentials are d...
The results of a systematic study of molecular properties by density functional theory (DFT) are presented and discussed. Equilibrium geometries, dipole moments, harmonic vibrat...
Abstract Compact contracted Gaussian basis sets introduced in the preceding article are tested for ab initio molecular calculations on molecules containing third‐row atoms (Na t...
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