Journal
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
Volume 13, Issue 6, Pages 2533-2549Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jctc.6b01118
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Funding
- Schweizerischer Nationalfonds (SNF) [200020_169120]
- Swiss National Science Foundation (SNF) [200020_169120] Funding Source: Swiss National Science Foundation (SNF)
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We present a matrix-product state (MPS)-based quadratically convergent density-matrix renormalization group self-consistent-field (DMRG-SCF) approach. Following a proposal by Werner and Knowles (J. Chem. Phys. 1985, 82, 5053), our DMRG-SCF algorithm is based on a direct minimization of an energy expression which is correct to second order with respect to changes in the molecular orbital basis. We exploit a simultaneous optimization of the MPS wave function and molecular orbitals in order to achieve quadratic convergence. In contrast to previously reported (augmented Hessian) Newton-Raphson and superconfiguration-interaction algorithms for DMRG-SCF, energy convergence beyond a quadratic scaling is possible in our ansatz. Discarding the set of redundant active-active orbital rotations, the DMRG-SCF energy converges typically within two to four cycles of the self-consistent procedure.
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