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Chemical Physics

Superoperator formalism in the perturbation theory of density operators obeying generalized liouville equations

K. Lendi

Published Feb 1, 1977• 13 citations
Publisher
DOI
10.1016/0301-0104(77)85121-5

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A direct approach for the generalized reduced Liouville equation of motion decoupling problem associated with open quantum systems within the superoperator formalism is presented. The procedure is based on inversion of the perturbation series for the energy representation of the density operator so as to obtain one for the proper self-energy fields that emerge as a consequence of the analytic character of the associated spectral representation. Thus, the perturbation series that arises from the iteration of the energy-dependent matrix elements hierarchy involved in the statistical operator allows, upon further expansion of the inverse of such series, to get formally exact expressions for the corrections to all orders of the self-energy fields. The lower order corrections of these fields are discussed in terms of resonant and nonresonant contributions. The present approach provides matrix equations that show the close relation between the environment effects represented by the self-energy fields and the relaxation kernel that drives the system–reservoir interaction. © 2000 John Wiley & Sons, Inc. Int J Quant Chem 79: 280–290, 2000
A generalized time-dependent perturbation theory is derived for superoperators. Instead of using the ``standard'' breakup of the Hamiltonian into a known zeroth order term and a correction, we use the approximate superpropagator to define the correction superoperator which is then used to obtain a series representation of the exact Liouville operator. The theory reduces to known limits and may be used for a perturbation expansion of classical Wigner and Husimi dynamics as well as for recent phase-space-based semiclassical approximations. The theory is demonstrated for a model quartic potential.
The Liouville equation differs from the von Neumann equation "only" by a characteristic superoperator. We demonstrate this for Hamiltonian dynamics, in general, and for the Jaynes-Cummings model, in particular. Employing superspace (instead of Hilbert space), we describe time evolution of density matrices in terms of path integrals, which are formally identical for quantum and classical mechanics. They only differ by the interaction contributing to the action. This allows us to import tools developed for Feynman path integrals, in order to deal with superoperators instead of quantum mechanical commutators in real time evolution. Perturbation theory is derived. Besides applications in classical statistical physics, the "classical path integral" and the parallel study of classical and quantum evolution indicate new aspects of (dynamically assisted) entanglement (generation). Our findings suggest to distinguish intra- from inter-space entanglement.