Partial atomic multipoles for internally consistent microelectrostatic calculations
| Autor: | Mateusz Snamina, Piotr Petelenz, Grzegorz Mazur |
|---|---|
| Rok vydání: | 2017 |
| Předmět: |
010304 chemical physics
Chemistry General Chemistry 010402 general chemistry 01 natural sciences 0104 chemical sciences Computational Mathematics Matrix (mathematics) Molecular solid Polarizability Yield (chemistry) Electric field 0103 physical sciences Molecule Charge carrier Atomic physics Solvent effects |
| Zdroj: | Journal of computational chemistry. 38(28) |
| ISSN: | 1096-987X |
| Popis: | An extension of the extant microelectrostatic methodologies, based on the concept of distributed generalized polarizability matrix derived from the Coupled Perturbed Hartree-Fock (CPHF) equations, is proposed for self-consistent calculation of charge carrier and charge-transfer (CT) state electrostatic energies in molecular solids, including the doped, defected and disordered ones. The CPHF equations are solved only once and the generalized molecular polarizability they yield enables low cost iterations that mutually adjust the molecular electronic distributions and the local electric field in which the molecules are immersed. The approach offers a precise picture of molecular charge densities, accounting for atomic partial multipoles up to order 2, which allows one to reproduce the recently reported large charge-quadrupole contributions to CT state energies in low-symmetry local environments. It is particularly well suited for repetitive calculations for large clusters (up to 300,000 atoms), and may potentially be useful for describing electrostatic solvent effects. © 2017 Wiley Periodicals, Inc. |
| Databáze: | OpenAIRE |
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