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Ensemble Generalized Kohn-Sham Theory: The Good, the Bad, and the Ugly

preprint
revised on 13.12.2020, 20:52 and posted on 15.12.2020, 08:51 by Tim Gould, Leeor Kronik
Two important extensions of Kohn-Sham (KS) theory are generalized KS theory and ensemble KS theory. The former allows for non-multiplicative potential operators and greatly facilitates practical calculations with advanced, orbital-dependent functionals. The latter allows for quantum ensembles and enables the treatment of, e.g., open systems and excited states. Here, we combine the two extensions, both formally and practically, first via an exact yet complicated formalism, then via a computationally tractable variant that involves a controlled approximation of ensemble "ghost interactions" by means of an iterative algorithm. The resulting formalism is illustrated using selected examples. This opens the door to the application of generalized KS theory in more challenging quantum scenarios and to the improvement of ensemble theories for the purpose of practical and accurate calculations.

Funding

Australian Research Council DP200100033

History

Email Address of Submitting Author

t.gould@griffith.edu.au

Institution

Griffith University

Country

Australia

ORCID For Submitting Author

0000-0002-7191-9124

Declaration of Conflict of Interest

No conflict of interest

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