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arXiv · 1904.05489

Tracking excited states in wave function optimization using density matrices and variational principles

Lan Nguyen Tran·Jacqueline A. R. Shea·Eric Neuscamman
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Abstract

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 based on energy ordering or a more direct generalization of the maximum overlap method. Furthermore, we provide evidence that this state-specific approach improves the performance of complete active space perturbation theory. 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.

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Lan Nguyen Tran, Jacqueline A. R. Shea, Eric Neuscamman. 2019-04-11. Tracking excited states in wave function optimization using density matrices and variational principles. https://arxiv.org/abs/1904.05489

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