The orbital-specific-virtual local coupled cluster singles and doubles method
We extend the orbital-specific-virtual tensor factorization, introduced for local Møller-Plesset perturbation theory in Ref. [J. Yang, Y. Kurashige, F. R. Manby and G. K. L. Chan, J. Chem. Phys. 134, 044123 (2011)10.1063/1.3528935], to local coupled cluster singles and doubles theory (OSV-LCCSD). The method is implemented by modifying an efficient projected-atomic-orbital local coupled cluster program (PAO-LCCSD) described recently, [H.-J. Werner and M. Schütz, J. Chem. Phys. 135, 144116 (2011)10.1063/1.3641642]. By comparison of both methods we find that the compact representation of the amplitudes in the OSV approach affords various advantages, including smaller computational time requirements (for comparable accuracy), as well as a more systematic control of the error through a single energy threshold. Overall, the OSV-LCCSD approach together with an MP2 correction yields small domain errors in practical calculations. The applicability of the OSV-LCCSD is demonstrated for molecules with up to 73 atoms and realistic basis sets (up to 2334 basis functions).
© 2012 American Institute of Physics. Received 7 January 2012; accepted 6 March 2012; published online 10 April 2012. G.K.C. acknowledges support from the Department of Energy (DOE), Office of Science Award DE-FG02-07ER46432. M.G.S. acknowledges support from the Deutsche Forschungsgemeinschaft (DFG). H.J.W. acknowledges support from the DFG within the SimTech Cluster of Excellence at the University of Stuttgart.
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