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Tracking Excited States in Wave Function Optimization Using Density Matrices and Variational Principles
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DOI：10.1021/acs.jctc.9b00351.png)
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摘要
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We present a method for finding individual excited states' energy stationary points in complete active space self-consistent field theory that is compatible with standard optimization methods and highly effective at overcoming difficulties due to root flipping and near-degeneracies. Inspired by both the maximum overlap method and recent progress in excited-state variational principles, our approach combines these ideas in order to track individual excited states throughout the orbital optimization process. In a series of tests involving root flipping, near-degeneracies, charge transfers, and double excitations, we show that this approach is more effective for state-specific optimization than either the naive selection of roots on the basis of energy ordering or a more direct generalization of the maximum overlap method. We provide evidence that this state-specific approach improves the performance of complete active space perturbation theory for vertical excitation energies. Furthermore, we find that the state-specific optimization can help avoid state-averaging-induced discontinuities on potential energy surfaces. With a simple implementation, a low cost, and compatibility with large active space methods, the approach is designed to be useful in a wide range of excited-state investigations.
Keyword:
SELF-CONSISTENT-FIELD
2ND-ORDER PERTURBATION-THEORY
POTENTIAL-ENERGY SURFACES
COUPLED-CLUSTER METHODS
QUANTUM MONTE-CARLO
CONICAL INTERSECTIONS
SCF METHOD
EFFICIENT
CASSCF
MULTIREFERENCE
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期刊
IF:
5.5
论文数:
1.1W
被引数:
5.4W
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