Conservation laws in coupled cluster dynamics at finite-temperature

We extend the finite-temperature Keldysh non-equilibrium coupled cluster theory (Keldysh-CC) [{\it J. Chem. Theory Comput.} \textbf{2019}, 15, 6137-6253] to include a time-dependent orbital basis. When chosen to minimize the action, such a basis restores local and global conservation laws (Ehrenfest...

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Bibliographic Details
Published in:arXiv.org 2021-06
Main Authors: Ruojing Peng, White, Alec F, Zhai, Huanchen, Chan, Garnet Kin-Lic
Format: Article
Language:English
Subjects:
Clusters
Conservation laws
Dynamics
Time dependence
Online Access:Get full text
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Summary:We extend the finite-temperature Keldysh non-equilibrium coupled cluster theory (Keldysh-CC) [{\it J. Chem. Theory Comput.} \textbf{2019}, 15, 6137-6253] to include a time-dependent orbital basis. When chosen to minimize the action, such a basis restores local and global conservation laws (Ehrenfest's theorem) for all one-particle properties, while remaining energy conserving for time-independent Hamiltonians. We present the time-dependent orbital-optimized coupled cluster doubles method (Keldysh-OCCD) in analogy with the formalism for zero-temperature dynamics, extended to finite temperatures through the time-dependent action on the Keldysh contour. To demonstrate the conservation property and understand the numerical performance of the method, we apply it to several problems of non-equilibrium finite-temperature dynamics: a 1D Hubbard model with a time-dependent Peierls phase, laser driving of molecular H\(_2\), driven dynamics in warm-dense silicon, and transport in the single impurity Anderson model.
ISSN:2331-8422
DOI:10.48550/arxiv.2106.02691