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arXiv:0803.4066 · Physical Review B

Dissipative two-electron transfer: A numerical renormalization group study

Sabine Tornow, R. Bulla, Frithjof B. Anders, Abraham Nitzan

Published Jul 18, 2008• 24 citations
arXivHTMLPDF

Abstract

We investigate nonequilibrium two-electron transfer in a model redox system represented by a two-site extended Hubbard model and embedded in a dissipative environment. The influence of the electron-electron interactions and the coupling to a dissipative bosonic bath on the electron transfer is studied in different temperature regimes. At high temperatures, Marcus transfer rates are evaluated, and at low temperatures, we calculate equilibrium and nonequilibrium population probabilities of the donor and acceptor with the nonperturbative numerical renormalization group approach. We obtain the nonequilibrium dynamics of the system prepared in an initial state of two electrons at the donor site and identify conditions under which the electron transfer involves one concerted two-electron step or two sequential single-electron steps. The rates of the sequential transfer depend nonmonotonically on the difference between the intersite and on-site Coulomb interaction, which become renormalized in the presence of the bosonic bath. If this difference is much larger than the hopping matrix element, the temperature as well as the reorganization energy, simultaneous transfer of both electrons between donor and acceptor can be observed.

DOI
10.1103/physrevb.78.035434

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We investigate nonequilibrium two-electron transfer in a model redox system represented by a two-site extended Hubbard model and embedded in a dissipative environment. The influence of the electron-electron interactions and the coupling to a dissipative bosonic bath on the electron transfer is studied in different temperature regimes. At high temperatures, Marcus transfer rates are evaluated, and at low temperatures, we calculate equilibrium and nonequilibrium population probabilities of the donor and acceptor with the nonperturbative numerical renormalization group approach. We obtain the nonequilibrium dynamics of the system prepared in an initial state of two electrons at the donor site and identify conditions under which the electron transfer involves one concerted two-electron step or two sequential single-electron steps. The rates of the sequential transfer depend nonmonotonically on the difference between the intersite and on-site Coulomb interaction, which become renormalized in the presence of the bosonic bath. If this difference is much larger than the hopping matrix element, the temperature as well as the reorganization energy, simultaneous transfer of both electrons between donor and acceptor can be observed.
We investigate electron transfer processes in donor-acceptor systems with a coupling of the electronic degrees of freedom to a common bosonic bath. The model allows to study many-particle effects and the influence of the local Coulomb interaction U between electrons on donor and acceptor sites. Using the non-perturbative numerical renormalization group approach we find distinct differences between the electron transfer characteristics in the single- and two-particle subspaces. We calculate the critical electron-boson coupling α c as a function of U and show results for density-density correlation functions in the whole parameter space. The possibility of many-particle (bipolaronic) and Coulomb-assisted transfer is discussed.
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Many-body physics is one very well suited field for testing quantum algorithms and for finding working heuristics on present quantum computers. We have investigated the non-equilibrium dynamics of one- and two-electron systems, which are coupled to an environment that introduces decoherence and dissipation. In our approach, the electronic system is represented in the framework of a two-site Hubbard model while the environment is modelled by a spin bath. To simulate the non-equilibrium population probabilities of the different states on a quantum computer we have encoded the electronic states and environmental degrees of freedom into qubits and ancilla qubits (bath), respectively. The total evolution time was divided into short time intervals, during which the system evolves. After each of these time steps, the system interacts with ancilla qubits representing the bath in thermal equilibrium. We have specifically studied spin baths leading to both, unital and non-unital dynamics of the electronic system and have found that electron correlations clearly enhance the electron transfer rates in the latter case. For short time periods, the simulation on the quantum computer is found to be in very good agreement with the exact results if error mitigation methods are applied. Our method to simulate also non-unitary time-evolution on a quantum computer can be well extended to simulate electronic systems in correlated spin baths as well as in bosonic and fermionic baths.
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.
We study the dissipative decay of states with a doubly occupied site in a two-electron Hubbard model, known as doublons. For the environment, we consider charge and current noise, which are modeled as a bosonic heat bath that couples to the on-site energies and the tunnel couplings, respectively. It turns out that the dissipative decay depends qualitatively on the type of environment, as for charge noise, the lifetime grows with the electron-electron interaction. For current noise, by contrast, doublons become increasingly unstable with larger interaction. Numerical studies within a Bloch-Redfield approach are complemented by analytical estimates for the decay rates. For typical quantum dot parameters, we predict doublon lifetimes up to 50 ns.
The nonequilibrium dynamics of correlated charge transfer along a one-dimensional chain in the presence of a phonon environment is investigated within a dissipative Hubbard model. For this generalization of the ubiquitous spin-boson model the crucial role of symmetries is analyzed in detail and corresponding invariant subspaces are identified. It is shown that the time evolution typically occurs in each of the disjunct subspaces independently leading, e.g., asymptotically to a non-Boltzmann equilibrium state. Based on these findings explicit results are obtained for two interacting electrons by means of a substantially improved real-time quantum Monte Carlo approach. In the incoherent regime an appropriate mapping of the many-body dynamics onto an isomorphic single particle motion allows for an approximate description of the numerical data in terms of rate equations. These results may lead to control schemes of charge transport in tailored quantum systems as, e.g., molecular chains or quantum dot arrays.