title: Cost reduction of high-order coupled-cluster methods via active-space and orbital transformation techniques.
abstract: We discuss several techniques which have the potential to decrease the computational expenses of high-order coupled-cluster (CC) methods with a reasonable loss in accuracy. In particular, the CC singles, doubles, and triples (CCSDT) as well as the CC singles, doubles, triples, and perturbative quadruples [CCSDT(Q)] methods are considered, which are frequently used in high-precision model chemistries for the calculation of iterative triples and quadruples corrections. First, we study the possibilities for using active spaces to decrease the computational costs. In this case, an active space is defined and some indices of cluster amplitudes are restricted to be in the space. Second, the application of transformed virtual orbitals is investigated. In this framework, to reduce the computation time the dimension of the properly transformed virtual one-particle space is truncated. We have found that the orbital transformation techniques outperform the active-space approaches. Using the transformation techniques, the computational time can be reduced in average by an order of magnitude without significant loss in accuracy. It is demonstrated that high-order CC calculations are possible for considerably larger systems than before using the implemented techniques.
authors: Department of Physical Chemistry and Materials Science, Budapest University of Technology and Economics, P.O.Box 91, H-1521 Budapest, Hungary.
authors: Zoltán
authors: Z
authors: Rolik
authors: Mihály
authors: M
authors: Kállay