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arXiv:2010.09838 · Physical Review Research

Open quantum systems beyond Fermi's golden rule: Diagrammatic expansion of the steady-state time-convolutionless master equations

Michael S. Ferguson, Oded Zilberberg, G. Blatter

Published May 19, 2021• 26 citations
arXivHTMLPDF

Abstract

Steady-state observables, such as occupation numbers and currents, are crucial experimental signatures in open quantum systems.The time-convolutionless (TCL) master equation, which is both exact and time-local, is an ideal candidate for the perturbative computation of such observables.We develop a diagrammatic approach to evaluate the steady-state TCL generator based on operators rather than superoperators.We obtain the steady-state occupation numbers, extend our formulation to the calculation of currents, and provide a simple physical interpretation of the diagrams.We further benchmark our method on a single noninteracting level coupled to Fermi reservoirs, where we recover the exact expansion to next-to-leading order.The low number of diagrams appearing in our formulation makes the extension to higher orders accessible.Combined, these properties make the steady-state time-convolutionless master equation an effective tool for the calculation of steady-state properties in open quantum systems.

DOI
10.1103/physrevresearch.3.023127

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Steady-state observables, such as occupation numbers and currents, are crucial experimental signatures in open quantum systems.The time-convolutionless (TCL) master equation, which is both exact and time-local, is an ideal candidate for the perturbative computation of such observables.We develop a diagrammatic approach to evaluate the steady-state TCL generator based on operators rather than superoperators.We obtain the steady-state occupation numbers, extend our formulation to the calculation of currents, and provide a simple physical interpretation of the diagrams.We further benchmark our method on a single noninteracting level coupled to Fermi reservoirs, where we recover the exact expansion to next-to-leading order.The low number of diagrams appearing in our formulation makes the extension to higher orders accessible.Combined, these properties make the steady-state time-convolutionless master equation an effective tool for the calculation of steady-state properties in open quantum systems.
We introduce simple diagrams and rules to calculate the exact time-local master equation for an arbitrary open quantum system interacting with a bath. In it, the time-convolutionless generator is expanded in the system-bath coupling to all orders, and the nthn\mathrm{th}nth-order contribution is expressed by the superoperators generated from the system operator in the system-bath coupling and the associated nnn-point nonequilibrium correlation functions of the environment operators. This theory generalizes previous attempts to obtain the time-convolutionless generator and provides a general framework to study the non-Markovian, nonequilibrium dynamics of open quantum systems.
The time-convolutionless master equation provides a general framework to model the non-Markovian dynamics of an open quantum system with a time-local generator. A diagrammatic representation is developed and proven for the perturbative expansion of the exact time-local generator for an open quantum system interacting with arbitrary environments. A truncation of the perturbation expansion leads to perturbative time-convolutionless quantum master equations. We further introduce a general iterative approach to construct nonperturbative approximations for the time-local generator as nested time-ordered exponential operators.
The time-convolutionless (TCL) quantum master equation provides a powerful tool to simulate reduced dynamics of a quantum system coupled to a bath. The key quantity in the TCL master equation is the so-called kernel or generator, which describes effects of the bath degrees of freedom. Since the exact TCL generators are usually hard to calculate analytically, most applications of the TCL generalized master equation have relied on approximate generators using second and fourth order perturbative expansions. By using the hierarchical equation of motion (HEOM) and extended HEOM methods, we present a new approach to calculating the exact TCL generator and its high order perturbative expansions. The new approach is applied to the spin-boson model with different sets of parameters, to investigate the convergence of the high order expansions of the TCL generator. We also discuss circumstances where the exact TCL generator becomes singular for the spin-boson model, and a model of excitation energy transfer in the Fenna-Matthews-Olson complex.
The time-convolutionless master equation provides a general framework to model non-Markovian dynamics of an open quantum system with a time-local generator. A diagrammatic representation is developed and proven for the perturbative expansion of the exact time-local generator for an open quantum system interacting with arbitrary environments. A truncation of the perturbation expansion leads to the perturbative time-convolutionless quantum master equations. We further introduce a nonperturbative approach that approximates the time-convolutionless generator as a nested time-ordered exponential function.
The non-Markovian dynamics of an open quantum system can be rigorously derived using the Feynman–Vernon influence functional approach. Although this formalism is exact, practical numerical implementations often require compromises. The time-convolutionless (TCL) master equation offers an exact framework, yet its application typically relies on a perturbative expansion of both the time forward and time backward state propagators. Due to the significant computational effort involved—and the scarcity of analytical solutions for most open quantum systems—the fourth-order perturbative TCL generator (TCL4) has only been benchmarked on a limited range of systems and parameter spaces. Recent advancements, however, have made the computation of TCL4 faster and more accessible. In this paper, we benchmark the TCL4 master equation against numerically exact methods for the biased spin-boson model. We focus on the regime near critical bath coupling where perturbative master equations are expected to become inaccurate. Our findings reveal that the TCL4 approach is most reliable at low temperatures and more efficient than the numerical exact methods. This study aims to delineate the conditions under which the TCL4 perturbative master equation enhances the accuracy of the TCL2.
We explore the performance of the time-convolutionless (TCL) projection operator technique using the Fano-Anderson model as a test case. Comparing the exact TCL master equation with an expansion in powers of the strength of the system-environment coupling, we analyze the transient dynamics as well as the steady-state behavior. For a Lorentzian spectral density we demonstrate that the dimensionless expansion parameter corresponds to the ratio of the environmental correlation time to the relaxation time of the system, and we derive the convergence radius for the TCL expansion, which is seen to depend on the ratio of detuning and width of the spectral density. We further study the quantum non-Markovianity of the model based on the evolution of the Bures distance between quantum states and how it is represented by the second and fourth order of the expansion. Our results highlight both the strengths and the limitations of the TCL formalism in capturing key features of open quantum systems and, in particular, the challenges of accurately describing strongly coupled systems and non-Markovian dynamics.