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Published November 13, 2018 | Supplemental Material + Submitted
Journal Article Open

A time-dependent formulation of coupled cluster theory for many-fermion systems at finite temperature

Abstract

We present a time-dependent formulation of coupled cluster theory. This theory allows for direct computation of the free energy of quantum systems at finite temperature by imaginary time integration and is closely related to the thermal cluster cumulant theory of Mukherjee and co-workers [ Chem. Phys. Lett. 1992, 192, 55−61; Phys. Rev. E 1993, 48, 3373−3389; Chem. Phys. Lett. 2001, 335, 281−288; Chem. Phys. Lett. 2002, 352, 63−69; Int. J. Mod. Phys. B 2003, 17, 5367−5377]. Our derivation of the finite-temperature theory highlights connections to perturbation theory and to zero-temperature coupled cluster theory. We show explicitly how the finite-temperature coupled cluster singles and doubles amplitude equations can be derived in analogy with the zero-temperature theory and how response properties can be efficiently computed using a variational Lagrangian. We discuss the implementation for realistic systems and showcase the potential utility of the method with calculations of the exchange correlation energy of the uniform electron gas under warm dense matter conditions.

Additional Information

© 2018 American Chemical Society. Received: July 26, 2018; Published: September 27, 2018. The authors would like to thank Jiajun Ren for helpful discussions. This work is supported by the U.S. Department of Energy, Office of Science, via Grant No. SC0018140. The authors declare no competing financial interest.

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Submitted - 1807.09961.pdf

Supplemental Material - ct8b00773_si_001.pdf

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