Dephasing in a Molecular Junction Viewed from a Time-Dependent and a Time-Independent Perspective

Rahman, Hasan; Karasch, Patrick; Ryndyk, Dmitry A.; Frauenheim, Thomas; Kleinekathöfer, Ulrich

doi:10.1021/acs.jpcc.9b00955

Cited by 7 publications

(5 citation statements)

References 84 publications

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“…In particular, through the spin-boson model, we demonstrated numerically and analytically that the decoherence effects due to a harmonic Ohmic environment (in the hightemperature pure-dephasing limit) can be mimicked by exponentially correlated colored Gaussian noise. This observation is consistent with a recent study [45] of the quantum transport properties of a molecular junction subject to vibrational dephasing that finds agreement between a fully quantum model (harmonic, Ohmic, pure-dephasing environment in the high temperature limit) and a model in which the thermal environment manifests itself in (exponentially correlated Gaussian) fluctuating site energies. A challenge in employing classical noise models for environments with more complicated spectral densities is to generate noise with the correct statistical properties.…”

Section: Discussionsupporting

confidence: 91%

“…According to Eq. Equation (45) suggests that for each spectral density there is a corresponding classical noise leading to the same pure-dephasing dynamics provided that an adequate algorithm to generate the stochastic process is identified. Here we exemplify the analysis with the widely used Ohmic environments with a Lorentz-Drude cutoff.…”

Section: Spin-boson Modelmentioning

confidence: 99%

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When can quantum decoherence be mimicked by classical noise?

Franco

2019

The Journal of Chemical Physics

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Quantum decoherence arises due to uncontrollable entanglement between a system with its environment. However the effects of decoherence are often thought of and modeled through a simpler picture in which the role of the environment is to introduce classical noise in the system's degrees of freedom. Here we establish necessary conditions that the classical noise models need to satisfy to quantitatively model the decoherence. Specifically, for pure-dephasing processes we identify well-defined statistical properties for the noise that are determined by the quantum many-point time correlation function of the environmental operators that enter into the system-bath interaction. In particular, for the exemplifying spin-boson problem with a Lorentz-Drude spectral density we show that the high-temperature quantum decoherence is quantitatively mimicked by colored Gaussian noise. In turn, for dissipative environments we show that classical noise models cannot describe decoherence effects due to spontaneous emission induced by a dissipative environment.These developments provide a rigorous platform to assess the validity of classical noise models of decoherence.

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Section: Discussionsupporting

confidence: 91%

Section: Spin-boson Modelmentioning

confidence: 99%

When can quantum decoherence be mimicked by classical noise?

Franco

2019

The Journal of Chemical Physics

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“…Quantum interference can be dynamically suppressed by the electron-phonon interaction, and the phase coherence destroyed by phonon scattering. Vibronic dephasing in molecular wires has been characterized in reference [484], where the effect of the thermal environment could be understood as fluctuating site energies of the wire.…”

Section: Electronic Transportmentioning

confidence: 99%

A many-body approach to transport in quantum systems: from the transient regime to the stationary state

Ridley

Talarico

Karlsson

et al. 2022

J. Phys. A: Math. Theor.

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We review one of the most versatile theoretical approaches to the study of time-dependent correlated quantum transport in nano-systems: the non-equilibrium Green's function (NEGF) formalism. Within this formalism, one can treat, on the same footing, inter-particle interactions, external drives and/or perturbations, and coupling to baths with a (piece-wise) continuum set of degrees of freedom. After a historical overview on the theory of transport in quantum systems, we present a modern introduction of the NEGF approach to quantum transport. We discuss the inclusion of inter-particle interactions using diagrammatic techniques, and the use of the so-called embedding and inbedding techniques which take the bath couplings into account non-perturbatively. In various limits, such as the non-interacting limit and the steady-state limit, we then show how the NEGF formalism elegantly reduces to well-known formulae in quantum transport as special cases. We then discuss non-equilibrium transport in general, for both particle and energy currents. Under the presence of a time-dependent drive -- encompassing pump--probe scenarios as well as driven quantum systems -- we discuss the transient as well as asymptotic behavior, and also how to use NEGF to infer information on the out-of-equilibrium system. As illustrative examples, we consider model systems general enough to pave the way to realistic systems. These examples encompass one- and two-dimensional electronic systems, systems with electron--phonon couplings, topological superconductors, and optically responsive molecular junctions where electron--photon couplings are relevant.

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“…Vibronic dephasing in molecular wires has been characterized in Ref. [440], where the effect of the thermal environment could be understood as fluctuating site energies of the wire.…”

Section: Electronic Transportmentioning

confidence: 99%

A many-body approach to transport in quantum systems: From the transient regime to the stationary state

Ridley,

Talarico,

Karlsson

et al. 2022

Preprint

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We review one of the most versatile theoretical approaches to the study of time-dependent correlated quantum transport in nano-systems: the non-equilibrium Green's function (NEGF) formalism. Within this formalism, one can treat, on the same footing, inter-particle interactions, external drives and/or perturbations, and coupling to baths with a (piece-wise) continuum set of degrees of freedom. After a historical overview on the theory of transport in quantum systems, we present a modern introduction of the NEGF approach to quantum transport. We discuss the inclusion of inter-particle interactions using diagrammatic techniques, and the use of the so-called embedding and inbedding techniques which take the bath couplings into account non-perturbatively. In various limits, such as the non-interacting limit and the steady-state limit, we then show how the NEGF formalism elegantly reduces to well-known formulae in quantum transport as special cases. We then discuss nonequilibrium transport in general, for both particle and energy currents. Under the presence of a time-dependent drive -encompassing pump-probe scenarios as well as driven quantum systems -we discuss the transient as well as asymptotic behavior, and also how to use NEGF to infer information on the out-of-equilibrium system.As illustrative examples, we consider model systems general enough to pave the way to realistic systems. These examples encompass one-and two-dimensional electronic systems, systems with electron-phonon couplings, topological superconductors, and optically responsive molecular junctions where electron-photon couplings are relevant.

show abstract

Dephasing in a Molecular Junction Viewed from a Time-Dependent and a Time-Independent Perspective

Cited by 7 publications

References 84 publications

When can quantum decoherence be mimicked by classical noise?

When can quantum decoherence be mimicked by classical noise?

A many-body approach to transport in quantum systems: from the transient regime to the stationary state

A many-body approach to transport in quantum systems: From the transient regime to the stationary state

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