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Journal ArticleDOI

Relativistic separable dual-space Gaussian pseudopotentials from H to Rn

15 Aug 1998-Physical Review B (American Physical Society)-Vol. 58, Iss: 7, pp 3641-3662
TL;DR: The relativistic dual-space Gaussian pseudopotential was introduced in this paper for the whole Periodic Table and a complete table of pseudopoetic parameters for all the elements from H to Rn.
Abstract: We generalize the concept of separable dual-space Gaussian pseudopotentials to the relativistic case. This allows us to construct this type of pseudopotential for the whole Periodic Table, and we present a complete table of pseudopotential parameters for all the elements from H to Rn. The relativistic version of this pseudopotential retains all the advantages of its nonrelativistic version. It is separable by construction, it is optimal for integration on a real-space grid, it is highly accurate, and, due to its analytic form, it can be specified by a very small number of parameters. The accuracy of the pseudopotential is illustrated by an extensive series of molecular calculations.
Citations
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Journal ArticleDOI
TL;DR: It is shown how derivatives of the GPW energy functional, namely ionic forces and the Kohn–Sham matrix, can be computed in a consistent way and the computational cost is scaling linearly with the system size, even for condensed phase systems of just a few tens of atoms.

4,047 citations

Journal ArticleDOI
30 Jan 2015-Science
TL;DR: An antisolvent vapor-assisted crystallization approach is reported that enables us to create sizable crack-free MAPbX3 single crystals with volumes exceeding 100 cubic millimeters, which enabled a detailed characterization of their optical and charge transport characteristics.
Abstract: The fundamental properties and ultimate performance limits of organolead trihalide MAPbX3 (MA = CH3NH3(+); X = Br(-) or I(-)) perovskites remain obscured by extensive disorder in polycrystalline MAPbX3 films. We report an antisolvent vapor-assisted crystallization approach that enables us to create sizable crack-free MAPbX3 single crystals with volumes exceeding 100 cubic millimeters. These large single crystals enabled a detailed characterization of their optical and charge transport characteristics. We observed exceptionally low trap-state densities on the order of 10(9) to 10(10) per cubic centimeter in MAPbX3 single crystals (comparable to the best photovoltaic-quality silicon) and charge carrier diffusion lengths exceeding 10 micrometers. These results were validated with density functional theory calculations.

3,939 citations


Cites methods from "Relativistic separable dual-space G..."

  • ...The plane-wave cutoff was 300 Ry, which is suitable for the Goedecker-Teter-Hutter pseudopotentials (32)....

    [...]

Journal ArticleDOI
TL;DR: An improvement to the grid‐based algorithm of Henkelman et al. for the calculation of Bader volumes is suggested, which more accurately calculates atomic properties as predicted by the theory of Atoms in Molecules, resulting in a more robust method of partitioning charge density among atoms in the system.
Abstract: An improvement to the grid-based algorithm of Henkelman et al. for the calculation of Bader volumes is suggested, which more accurately calculates atomic properties as predicted by the theory of Atoms in Molecules. The CPU time required by the improved algorithm to perform the Bader analysis scales linearly with the number of interatomic surfaces in the system. The new algorithm corrects systematic deviations from the true Bader surface, calculated by the original method and also does not require explicit representation of the interatomic surfaces, resulting in a more robust method of partitioning charge density among atoms in the system. Applications of the method to some small systems are given and it is further demonstrated how the method can be used to define an energy per atom in ab initio calculations.

2,999 citations

Journal ArticleDOI
TL;DR: A library of Gaussian basis sets that has been specifically optimized to perform accurate molecular calculations based on density functional theory and can be used in first principles molecular dynamics simulations and is well suited for linear scaling calculations.
Abstract: We present a library of Gaussian basis sets that has been specifically optimized to perform accurate molecular calculations based on density functional theory. It targets a wide range of chemical environments, including the gas phase, interfaces, and the condensed phase. These generally contracted basis sets, which include diffuse primitives, are obtained minimizing a linear combination of the total energy and the condition number of the overlap matrix for a set of molecules with respect to the exponents and contraction coefficients of the full basis. Typically, for a given accuracy in the total energy, significantly fewer basis functions are needed in this scheme than in the usual split valence scheme, leading to a speedup for systems where the computational cost is dominated by diagonalization. More importantly, binding energies of hydrogen bonded complexes are of similar quality as the ones obtained with augmented basis sets, i.e., have a small (down to 0.2 kcal/mol) basis set superposition error, and the monomers have dipoles within 0.1 D of the basis set limit. However, contrary to typical augmented basis sets, there are no near linear dependencies in the basis, so that the overlap matrix is always well conditioned, also, in the condensed phase. The basis can therefore be used in first principles molecular dynamics simulations and is well suited for linear scaling calculations.

2,700 citations

Journal ArticleDOI
TL;DR: ABINITv3.0 is described, in which freedom of sources, reliability, portability, and self-documentation are emphasised, in the development of a sophisticated plane-wave pseudopotential code.

2,596 citations

References
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Book
01 Jan 1989
TL;DR: In this paper, a review of current studies in density functional theory and density matrix functional theory is presented, with special attention to the possible applications within chemistry, including the concept of an atom in a molecule, calculation of electronegativities from the Xα method, pressure, Gibbs-Duhem equation, Maxwell relations and stability conditions.
Abstract: Current studies in density functional theory and density matrix functional theory are reviewed, with special attention to the possible applications within chemistry. Topics discussed include the concept of electronegativity, the concept of an atom in a molecule, calculation of electronegativities from the Xα method, the concept of pressure, Gibbs-Duhem equation, Maxwell relations, stability conditions, and local density functional theory.

14,008 citations

Book
01 Jan 1979

3,903 citations

BookDOI
TL;DR: In this paper, the authors present an approach to calculate the energy levels of Diatomic molecules in terms of the number of excited states in the molecules and the lifetime of these states.
Abstract: 1. Introduction.- 2. Units of Physical Quantities.- 2.1 Systems of Units in Physics.- 2.2 Fundamental Physical Constants.- 2.3 Systems of Units Based on "Natural Standards".- 2.4 Tables of Conversion Factors.- I Atoms and Atomic Ions.- 3. Isotopic Composition, Atomic Mass Table and Atomic Weights of the Elements.- 3.1 Parameters of Stable and Long-Lived Isotopes.- 3.2 Atomic Weights of the Elements and Atomic Mass Table.- 4. Structure of Atomic Electron Shells.- 4.1 Electron Configurations and Ground-State Terms.- 4.2 The Periodic Table.- 4.3 Parameters of Wavefunctions for Valence Electrons in Atoms, Positive and Negative Ions.- 5. Energetics of Neutral Atoms.- 5.1 Ionization Potentials of Atoms.- 5.2 Quantum Defects of Atomic Rydberg States.- 5.3 Fine-Structure Splitting of Atomic Energy Levels.- 5.4 Hyperfine Structure of Atomic Energy Levels.- 5.5 Isotope Shifts of Low-Lying Atomic Levels.- 5.6 Atoms in Static Electric and Magnetic Fields. Atomic Polarizabilities and Magnetic Susceptibilities.- 6. Energetics of Atomic Ions.- 6.1 Ionization Potentials of Atomic Ions.- 6.2 Electron Affinities of Atoms.- 6.3 Energy Levels of Multiply Charged Atomic Ions.- 7. Spectroscopic Characteristics of Neutral Atoms.- 7.1 Low-Lying Atomic Terms.- 7.2 Diagrams of Atomic Energy Levels and Grotrian Diagrams.- 7.3 Atomic Oscillator Strengths in Absorption.- 7.4 Lifetimes of Resonant Excited States in Atoms.- 7.5 Energy Levels and Lifetimes for Metastable States in Atoms.- 7.6 Lifetimes of Atomic Rydberg States.- 8. Spectroscopic Characteristics of Atomic Positive Ions.- 8.1 Low-Lying Terms of Singly Ionized Atoms.- 8.2 Lifetimes of Resonant Excited States in Atomic Ions.- 8.3 Energy Levels and Lifetimes for Metastable States in Singly Ionized Atoms.- 8.4 Optical Parameters of Multiply Charged Atomic Ions.- II Molecules and Molecular Ions.- 9. Interaction Potentials Between Atomic and Molecular Species.- 9.1 Van der Waals Coefficients for Interatomic Multipole Interactions.- 9.2 Long-Range Exchange Interactions of Atoms.- 9.3 Short-Range Repulsive Interactions Between Atomic and Molecular Species.- 10. Diatomic Molecules.- 10.1 Electron Configurations of Diatomic Molecules.- 10.2 Asymptotic Parameters of Wavefunctions for Valence Electrons in Diatomic Molecules.- 10.3 Spectroscopic Constants of Diatomic Molecules.- 10.4 Potential Energy Curves.- 10.5 Ionization Potentials of Diatomic Molecules.- 10.6 Dissociation Energies of Diatomic Molecules.- 10.7 Lifetimes of Excited Electron States in Diatomic Molecules.- 10.8 Parameters of Excimer Molecules.- 10.9 Einstein Coefficients for Spontaneous Emission from Vibrationally Excited Diatomic Molecules.- 11. Diatomic Molecular Ions.- 11.1 Electron Configurations and Asymptotic Parameters of Wavefunctions for Valence Electrons in Diatomic Molecular Ions.- 11.2 Spectroscopic Constants of Diatomic Molecular Ions.- 11.3 Dissociation Energies of Diatomic Molecular Ions.- 11.4 Electron Affinities of Diatomic Molecules.- 11.5 Proton Affinities of Atoms.- 11.6 Lifetimes of Excited Electron States in Diatomic Molecular Ions.- 12. Van der Waals Molecules.- 12.1 Potential Well Parameters of Van der Waals Molecules.- 12.2 Potential Well Parameters of Van der Waals Molecular Ions.- 12.3 Ionization Potentials of Van der Waals Molecules.- 13. Polyatomic Molecules.- 13.1 Constants of Triatomic Molecules.- 13.2 Ionization Potentials of Polyatomic Molecules.- 13.3 Bond Dissociation Energies of Polyatomic Molecules.- 13.4 Lifetimes of Vibrationally Excited Polyatomic Molecules.- 14. Polyatomic Molecular Ions.- 14.1 Bond Dissociation Energies of Complex Positive Ions.- 14.2 Bond Dissociation Energies of Complex Negative Ions.- 14.3 Electron Affinities of Polyatomic Molecules.- 14.4 Proton Affinities of Molecules.- 15. Electrical Properties of Molecules.- 15.1 Dipole Moments of Molecules.- 15.2 Molecular Polarizabilities.- 15.3 Quadrupole Moments of Molecules.- Mathematical Appendices.- A. Coefficients of Fractional Parentage.- B. Clebsch-Gordan Coefficients.

1,688 citations

Book ChapterDOI
01 Jan 1995

42 citations