English

Approximate analytical gradients and nonadiabatic couplings for the state-average density matrix renormalization group self-consistent field method

Chemical Physics 2020-02-18 v2 Strongly Correlated Electrons Computational Physics Quantum Physics

Abstract

We present an approximate scheme for analytical gradients and nonadiabatic couplings for calculating state-average density matrix renormalization group self-consistent-field wavefunction. Our formalism follows closely the state-average complete active space self-consistent-field (SA-CASSCF) \emph{ansatz}, which employs a Lagrangian, and the corresponding Lagrange multipliers are obtained from a solution of the coupled-perturbed CASSCF (CP-CASSCF) equations. We introduce a definition of the matrix product state (MPS) Lagrange multipliers based on a single-site tensor in a mixed-canonical form of the MPS, such that a sweep procedure is avoided in the solution of the CP-CASSCF equations. We apply our implementation to the optimization of a conical intersection in 1,2-dioxetanone, where we are able to fully reproduce the SA-CASSCF result up to arbitrary accuracy.

Keywords

Cite

@article{arxiv.1905.01558,
  title  = {Approximate analytical gradients and nonadiabatic couplings for the state-average density matrix renormalization group self-consistent field method},
  author = {Leon Freitag and Yingjin Ma and Alberto Baiardi and Stefan Knecht and Markus Reiher},
  journal= {arXiv preprint arXiv:1905.01558},
  year   = {2020}
}

Comments

17 pages, 3 figures, 2 tables

R2 v1 2026-06-23T08:57:07.859Z