Purification of correlated reduced density matrices.

Abstract

The notion of purification is generalized to treat correlated reduced density matrices. Traditionally, purification denotes the process by which a one-particle reduced density matrix (1-RDM) is made idempotent, that is, its eigenvalues are mapped to either 0 or 1. Purification of correlated RDMs is defined as the iterative process by which an arbitrary RDM is forced to satisfy several necessary N-representability conditions. Using the unitary decomposition of RDMs and the positivity conditions, we develop an algorithm to purify the 2-RDM. The algorithm is applied within the solution of the contracted Schrödinger equation CSE for the 2-RDM [D. A. Mazziotti, Phys. Rev. A 57, 4219 (1998)]. Previous attempts to solve the CSE by powerlike methods have frequently produced divergent energies, but we show that the purification process eliminates the divergent behavior for systematic and reliable convergence of the contracted power method to the N-particle energy.