A method of orbital analysis for large-scale first-principles simulations
- Advanced Materials Laboratory, Nissan Research Center, Nissan Motor Co., Ltd., 1 Natsushima-cho, Yokosuka, Kanagawa 237-8523 (Japan)
- Nanosystem Research Institute, National Institute of Advanced Industrial Science and Technology (AIST), Tsukuba, Ibaraki 305-8568 (Japan)
- Research Center for Simulation Science (RCSS), Japan Advanced Institute of Science and Technology (JAIST), 1-1 Asahidai, Nomi, Ishikawa 923-1292 (Japan)
An efficient method of calculating the natural bond orbitals (NBOs) based on a truncation of the entire density matrix of a whole system is presented for large-scale density functional theory calculations. The method recovers an orbital picture for O(N) electronic structure methods which directly evaluate the density matrix without using Kohn-Sham orbitals, thus enabling quantitative analysis of chemical reactions in large-scale systems in the language of localized Lewis-type chemical bonds. With the density matrix calculated by either an exact diagonalization or O(N) method, the computational cost is O(1) for the calculation of NBOs associated with a local region where a chemical reaction takes place. As an illustration of the method, we demonstrate how an electronic structure in a local region of interest can be analyzed by NBOs in a large-scale first-principles molecular dynamics simulation for a liquid electrolyte bulk model (propylene carbonate + LiBF{sub 4})
- OSTI ID:
- 22311383
- Journal Information:
- Journal of Chemical Physics, Vol. 140, Issue 24; Other Information: (c) 2014 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA); ISSN 0021-9606
- Country of Publication:
- United States
- Language:
- English
Similar Records
Accelerating Atomic Orbital-based Electronic Structure Calculation via Pole Expansion plus Selected Inversion
Real-space formulation of the stress tensor for O(N) density functional theory: Application to high temperature calculations