Density-matrix renormalization group algorithm with multi-level active space

The density-matrix renormalization group (DMRG) method, which can deal with a large active space composed of tens of orbitals, is nowadays widely used as an efficient addition to traditional complete active space (CAS)-based approaches. In this paper, we present the DMRG algorithm with a multi-level (ML) control of the active space based on chemical intuition-based hierarchical orbital ordering, which is called as ML-DMRG with its self-consistent field (SCF) variant ML-DMRG-SCF. Ground and excited state calculations of H2O, N-2, indole, and Cr-2 with comparisons to DMRG references using fixed number of kept states (M) illustrate that ML-type DMRG calculations can obtain noticeable efficiency gains. It is also shown that the orbital re-ordering based on hierarchical multiple active subspaces may be beneficial for reducing computational time for not only ML-DMRG calculations but also DMRG ones with fixed M values. (C) 2015 AIP Publishing LLC.