Journal
CHEMICAL PHYSICS
Volume 391, Issue 1, Pages 130-142Publisher
ELSEVIER
DOI: 10.1016/j.chemphys.2011.03.014
Keywords
Time-dependent density functional theory; Open quantum systems; Relaxation and decoherence; Lindblad master equation
Funding
- NSF [PHY-0835713]
- Camille and Henry Dreyfus Teacher-Scholar award
- Sloan Research Fellowship
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The dissipative dynamics of many-electron systems interacting with a thermal environment has remained a long-standing challenge within time-dependent density functional theory (TDDFT). Recently, the formal foundations of open quantum systems time-dependent density functional theory (OQS-TDDFT) within the master equation approach were established. It was proven that the exact time-dependent density of a many-electron open quantum system evolving under a master equation can be reproduced with a closed (unitarily evolving) and non-interacting Kohn-Sham system. This potentially offers a great advantage over previous approaches to OQS-TDDFT, since with suitable functionals one could obtain the dissipative open-systems dynamics by simply propagating a set of Kohn-Sham orbitals as in usual TDDFT. However, the properties and exact conditions of such open-systems functionals are largely unknown. In the present article, we examine a simple and exactly-solvable model open quantum system: one electron in a harmonic well evolving under the Lindblad master equation. We examine two different representitive limits of the Lindblad equation (relaxation and pure dephasing) and are able to deduce a number of properties of the exact OQS-TDDFT functional. Challenges associated with developing approximate functionals for many-electron open quantum systems are also discussed. (C) 2011 Elsevier B. V. All rights reserved.
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