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Phys. Rev. B 76, 195316 (2007) [21 pages]

Nonequilibrium quantum dissipation in spin-fermion systems

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Dvira Segal* and David R. Reichman
Department of Chemistry, Columbia University, 3000 Broadway, New York, New York 10027, USA

Andrew J. Millis
Department of Physics, Columbia University, 538 West 120th Street, New York, New York 10027, USA

Received 30 August 2007; published 16 November 2007

Dissipative processes in nonequilibrium many-body systems are fundamentally different than their equilibrium counterparts. Such processes are of great importance for the understanding of relaxation in single-molecule devices. As a detailed case study, we investigate here a generic spin-fermion model, where a two-level system couples to two metallic leads with different chemical potentials. We present results for the spin relaxation rate in the nonadiabatic limit for an arbitrary coupling to the leads using both analytical and exact numerical methods. The nonequilibrium dynamics is reflected by an exponential relaxation at long times and via complex phase shifts, leading in some cases to an “antiorthogonality” effect. In the limit of strong system-lead coupling at zero temperature we demonstrate the onset of a Marcus-like Gaussian decay with voltage difference activation. This is analogous to the equilibrium spin-boson model, where at strong coupling and high temperatures, the spin excitation rate manifests temperature activated Gaussian behavior. We find that there is no simple linear relationship between the role of the temperature in the bosonic system and a voltage drop in a nonequilibrium electronic case. The two models also differ by the orthogonality-catastrophe factor existing in a fermionic system, which modifies the resulting line shapes. Implications for current characteristics are discussed. We demonstrate the violation of pairwise Coulomb gas behavior for strong coupling to the leads. The results presented in this paper form the basis of an exact, nonperturbative description of steady-state quantum dissipative systems.

© 2007 The American Physical Society

URL:
http://link.aps.org/doi/10.1103/PhysRevB.76.195316
DOI:
10.1103/PhysRevB.76.195316
PACS:
73.63.−b, 03.65.Yz, 05.60.Gg, 72.10.Fk

*Corresponding author. Present address: Chemical Physics Theory Group, Department of Chemistry, University of Toronto, Ontario, Canada M5S 3H6. dsegal@chem.utoronto.ca