Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Log inSign up
Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Blog
Job Board
Q3AS

© 2026 Aqora Quantum S.A.S.

TermsPrivacyLegal Notice

arXiv:cond-mat/0508098 · Physical Review Letters

Nonequilibrium Dynamics of Correlated Electron Transfer in Molecular Chains

Lothar Mühlbacher, Joachim Ankerhold, A. Komnik

Published Nov 23, 2005• 25 citations
arXivHTMLPDF

Abstract

The relaxation dynamics of correlated electron transport along molecular chains is studied based on a substantially improved numerically exact path integral Monte Carlo approach. As an archetypical model, we consider a Hubbard chain containing two interacting electrons coupled to a bosonic bath. For this generalization of the ubiquitous spin-boson model, non-Boltzmann equilibrium distributions are found for many-body states. By mapping the multiparticle dynamics onto an isomorphic single particle motion, this phenomenon is shown to be sensitive to particle statistics and, due to its robustness, allows for new control schemes in designed quantum aggregates.

DOI
10.1103/physrevlett.95.220404

Related papers

Nonequilibrium many-body dynamics along a dissipative Hubbard chain: Symmetries and quantum Monte Carlo simulations

Lothar Mühlbacher, Joachim Ankerhold

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.

arXiv:cond-mat/0605166•Physical Review B•Oct 12, 2006•3 citations

Correlated charge transfer along molecular chains

Lothar Mühlbacher, Joachim Ankerhold

The nonequilibrium dynamics of charges along one-dimensional tight-binding lattices subject to a vibronic background is analyzed in the two-particle sector of a dissipative Hubbard model. The role of symmetries for distinguishable fermions with opposite spins and for indistinguishable ones with polarized spins is revealed and is shown to cause transfer dynamics with non-Boltzmann types of asymptotic distributions. Explicit results are obtained within an improved path integral Monte Carlo approach and are compared against an approximate description in terms of rate equations.

New Journal of Physics•Jun 30, 2008•2 citations

Dissipative two-electron transfer: A numerical renormalization group study

Sabine Tornow, R. Bulla, Frithjof B. Anders +1 more

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.

arXiv:0803.4066•Physical Review B•Jul 18, 2008•24 citations

A theory of electron baths: One-electron system dynamics

H. Keith McDowell

The second-quantized, many-electron, atomic, and molecular Hamiltonian is partitioned both by the identity or labeling of the spin orbitals and by the dynamics of the spin orbitals into a system coupled to a bath. The electron bath is treated by a molecular time scale generalized Langevin equation approach designed to include one-electron dynamics in the system dynamics. The bath is formulated as an equivalent chain of spin orbitals through the introduction of equivalent-chain annihilation and creation operators. Both the dynamics and the quantum grand canonical statistical properties of the electron bath are examined. Two versions for the statistical properties of the bath are pursued. Using a weak bath assumption, a bath statistical average is defined which allows one to achieve a reduced dynamics description of the electron system which is coupled to the electron bath. In a strong bath assumption effective Hamiltonians are obtained which reproduce the dynamics of the bath and which lead to the same results as found in the weak bath assumption. The effective (but exact) Hamiltonian is found to be a one-electron Hamiltonian. A reduced dynamics equation of motion for the system population matrix is derived and found to agree with a previous version. This equation of motion is useful for studying electron transfer in the system when coupled to an electron bath.

The Journal of Chemical Physics•Feb 1, 1992•2 citations

Non-Equilibrium Dynamics of a Dissipative Two-Site Hubbard Model Simulated on the IBM Quantum Computer

Sabine Tornow, Wolfgang Gehrke, U. Helmbrecht

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.

•Nov 22, 2020•3 citations

Non-equilibrium dynamics of a dissipative two-site Hubbard model simulated on IBM quantum computers

Sabine Tornow, Wolfgang Gehrke, U. Helmbrecht

Abstract 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.

arXiv:2011.11059•Journal of Physics A Mathematical and Theoretical•Apr 29, 2022•15 citations
The relaxation dynamics of correlated electron transport along molecular chains is studied based on a substantially improved numerically exact path integral Monte Carlo approach. As an archetypical model, we consider a Hubbard chain containing two interacting electrons coupled to a bosonic bath. For this generalization of the ubiquitous spin-boson model, non-Boltzmann equilibrium distributions are found for many-body states. By mapping the multiparticle dynamics onto an isomorphic single particle motion, this phenomenon is shown to be sensitive to particle statistics and, due to its robustness, allows for new control schemes in designed quantum aggregates.
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.
The nonequilibrium dynamics of charges along one-dimensional tight-binding lattices subject to a vibronic background is analyzed in the two-particle sector of a dissipative Hubbard model. The role of symmetries for distinguishable fermions with opposite spins and for indistinguishable ones with polarized spins is revealed and is shown to cause transfer dynamics with non-Boltzmann types of asymptotic distributions. Explicit results are obtained within an improved path integral Monte Carlo approach and are compared against an approximate description in terms of rate equations.
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.
The second-quantized, many-electron, atomic, and molecular Hamiltonian is partitioned both by the identity or labeling of the spin orbitals and by the dynamics of the spin orbitals into a system coupled to a bath. The electron bath is treated by a molecular time scale generalized Langevin equation approach designed to include one-electron dynamics in the system dynamics. The bath is formulated as an equivalent chain of spin orbitals through the introduction of equivalent-chain annihilation and creation operators. Both the dynamics and the quantum grand canonical statistical properties of the electron bath are examined. Two versions for the statistical properties of the bath are pursued. Using a weak bath assumption, a bath statistical average is defined which allows one to achieve a reduced dynamics description of the electron system which is coupled to the electron bath. In a strong bath assumption effective Hamiltonians are obtained which reproduce the dynamics of the bath and which lead to the same results as found in the weak bath assumption. The effective (but exact) Hamiltonian is found to be a one-electron Hamiltonian. A reduced dynamics equation of motion for the system population matrix is derived and found to agree with a previous version. This equation of motion is useful for studying electron transfer in the system when coupled to an electron bath.
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.
Abstract 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.