Welcome to the new version of CaltechAUTHORS. Login is currently restricted to library staff. If you notice any issues, please email coda@library.caltech.edu
Published July 28, 2021 | Submitted + Published + Supplemental Material
Journal Article Open

Conservation laws in coupled cluster dynamics at finite temperature

Abstract

We extend the finite-temperature Keldysh non-equilibrium coupled cluster theory (Keldysh-CC) [A. F. White and G. K.-L. Chan, J. Chem. Theory Comput. 15, 6137–6253 (2019)] 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 Keldysh orbital-optimized coupled cluster doubles method 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 H₂, driven dynamics in warm-dense silicon, and transport in the single impurity Anderson model.

Additional Information

© 2021 Published under an exclusive license by AIP Publishing. Submitted: 7 June 2021; Accepted: 1 July 2021; Published Online: 26 July 2021. This work was supported by the U.S. Department of Energy, Office of Science, via Grant No. DE-SC0018140. Benchmarks generated by DMRG used PyBlock3, a code developed with support from the U.S. National Science Foundation under Grant No. CHE-2102505. G.K.C. thanks Emanuel Gull for discussions. G.K.C. is a Simons Investigator in Physics and is part of the Simons Collaboration on the Many-Electron Problem. Authors' Contributions: R.P. and A.F.W. contributed equally to this work.

Attached Files

Published - 5.0059257.pdf

Submitted - 2106.02691.pdf

Supplemental Material - supplemental_material_conservation_laws_in_coupled_cluster_dynamics_at_finite_temperature_1.pdf

Files

supplemental_material_conservation_laws_in_coupled_cluster_dynamics_at_finite_temperature_1.pdf
Files (5.4 MB)
Name Size Download all
md5:e470e9789f6ac7ebe8c3f3eae53be58e
68.0 kB Preview Download
md5:c503465b92327222d4dc884918626689
718.8 kB Preview Download
md5:64c1157f360c0b90e061e93e384b0beb
4.6 MB Preview Download

Additional details

Created:
August 20, 2023
Modified:
October 23, 2023