Parallel Implementation of Gamma-Point Pseudopotential Plane-Wave DFT with Exact Exchange
One of the more persistent failures of conventional density functional theory (DFT) methods has been their failure to yield localized charge states such as polarons, excitons and solitons in solid-state and extended systems. It has been suggested that conventional DFT functionals, which are not self-interaction free, tend to favor delocalized electronic states since self-interaction creates a Coulomb barrier to charge localization. Pragmatic approaches in which the exchange correlation functionals are augmented with small amount of exact exchange (hybrid-DFT, e.g. B3LYP and PBE0) have shown promise in localizing charge states and predicting accurate band gaps and reaction barriers. We have developed a parallel algorithm for implementing exact exchange into pseudopotential plane-wave density functional theory and we have implemented it in the NWChem program package. The technique developed can readily be employed in plane-wave DFT programs. Furthermore, atomic forces and stresses are straightforward to implement, making it applicable to both confined and extended systems, as well as to Car-Parrinello ab initio molecular dynamic simulations. This method has been applied to several systems for which conventional DFT methods do not work well, including calculations for band gaps in oxides and the electronic structure of a charge trapped state in the Fe(II) containing mica, annite.
- Research Organization:
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
- Sponsoring Organization:
- USDOE
- DOE Contract Number:
- AC05-76RL01830
- OSTI ID:
- 1002156
- Report Number(s):
- PNNL-SA-64272; 30995; 29990; 2573b; 25714; 1417c; 2392; 20900; 18590; 9597; 3564a; KJ0101010; TRN: US1100485
- Journal Information:
- Journal of Computational Chemistry, 32(1):54-69, Vol. 32, Issue 1; ISSN 0192-8651
- Country of Publication:
- United States
- Language:
- English
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Related Subjects
ALGORITHMS
CHARGE STATES
COULOMB FIELD
ELECTRONIC STRUCTURE
EXCITONS
FUNCTIONALS
IMPLEMENTATION
MICA
OXIDES
POLARONS
SOLITONS
STRESSES
DFT
Coulomb
pseudopotential
NWChem
calculations
excitons
polarons
solitons
hybrid DFT
parallel algorithms
exact exchange
pseudopotential plane-wave DFT
Environmental Molecular Sciences Laboratory