Journal
JOURNAL OF CHEMICAL PHYSICS
Volume 137, Issue 10, Pages -Publisher
AMER INST PHYSICS
DOI: 10.1063/1.4747538
Keywords
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Funding
- German Academic Exchange Service (DAAD)
- U.S. National Science Foundation (NSF) [NSF-OCI-0904972]
- U.S. National Science Foundation (CAREER Award) [CHE-0847295]
- U.S. National Science Foundation (CRIF:MU Award) [CHE-0741927]
- U.S. National Science Foundation (SI2-SSI Award) [OCI-1047696]
- Direct For Mathematical & Physical Scien
- Division Of Chemistry [0847295] Funding Source: National Science Foundation
- Office of Advanced Cyberinfrastructure (OAC)
- Direct For Computer & Info Scie & Enginr [0904972] Funding Source: National Science Foundation
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We present an approach to compute accurate correlation energies for atoms and molecules using an adaptive discontinuous spectral-element multiresolution representation for the two-electron wave function. Because of the exponential storage complexity of the spectral-element representation with the number of dimensions, a brute-force computation of two-electron (six-dimensional) wave functions with high precision was not practical. To overcome the key storage bottlenecks we utilized (1) a low-rank tensor approximation (specifically, the singular value decomposition) to compress the wave function, and (2) explicitly correlated R12-type terms in the wave function to regularize the Coulomb electron-electron singularities of the Hamiltonian. All operations necessary to solve the Schrodinger equation were expressed so that the reconstruction of the full-rank form of the wave function is never necessary. Numerical performance of the method was highlighted by computing the first-order Moller-Plesset wave function of a helium atom. The computed second-order Moller-Plesset energy is precise to similar to 2 microhartrees, which is at the precision limit of the existing general atomic-orbital-based approaches. Our approach does not assume special geometric symmetries, hence application to molecules is straightforward. (C) 2012 American Institute of Physics. [http://dx.doi.org/10.1063/1.4747538]
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