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arXiv:2604.22010 · The Journal of Chemical Physics

Expansion of time-convolutionless non-Markovian quantum master equations: A case study using the Fano-Anderson model

Tim Alhäuser, Heinz-Peter Breuer

quant-phSubmitted Apr 23, 2026• Announced Apr 27, 2026• 0 citations
arXivHTMLPDF

Abstract

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.

Journal reference
J. Chem. Phys. 164, 164110 (2026)
DOI
10.1063/5.0323348
Comments
13 pages, 13 figures

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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.
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 spin-boson model is a widely used model for understanding the properties of a two-level open quantum system. Accurately describing its dynamics often requires going beyond the weak system-environment coupling approximation. However, calculating the higher-order generators of such a dynamics, with a system-environment coupling that is not too weak, has been known to be challenging, both numerically and analytically. This work presents the analytical derivation of the complete fourth-order time-convolutionless (TCL) generator for a generic spin-boson model, accurate up to 4th order in the system-environment coupling parameter, under the assumption that the environmental spectral density is an odd function of frequency. In the case of a semiconductor double-quantum-dot system, our results reveal corrections to the dynamics that may become physically significant in some parameter regimes. Furthermore, we report that the widely used second-order TCL master equation tends to overestimate the non-Markovianity of a dynamics over a large parameter regime. Within the regime of its applicability, our results provide a computational advantage over numerically exact techniques. The accuracy of the fourth-order TCL generator is rigorously benchmarked against specialized analytical calculations done for the Ohmic spectral density with Drude cutoff and against the numerically exact Hierarchical Equations of Motion technique.
Perturbative master equations are essential for modeling open quantum systems but often exhibit late-time divergences when environmental correlations decay algebraically. In this work, we analyze the time-convolutionless (TCL) master equation expanded to order TCL2n{\mathrm{TCL}}_{2n}TCL2n​ and demonstrate that, while van Kampen's cumulants suppress early-time secular growth, they ultimately diverge at long times. To overcome this, we introduce a resummation technique based on the Hadamard trick, which incorporates time integrals directly into the bath's spectral density via elementwise multiplication. This approach establishes a maximum expansion order, ${n}_{\text{max}}=\ensuremath{\lceil}s+1\ensuremath{\rceil}$, and defines a precision limit of the asymptotic states of $O({\ensuremath{\lambda}}^{2\ensuremath{\lceil}s\ensuremath{\rceil}})$, where sss is the power-law exponent and $\ensuremath{\lambda}$ is the weak-coupling constant. The resummed master equation features renormalized Bohr frequencies that capture decoherence and spectral overlap effects. In the unbiased spin-boson model, this results in an inflation of the generator at a temperature-independent rate equal to the decoherence rate ${\ensuremath{\nu}}_{2}$ and a finite validity time ${t}_{L}\ensuremath{\approx}(s+1)/{\ensuremath{\nu}}_{2}$. For exponentially decaying correlations, the method recovers a proper Markovian limit below a critical coupling threshold.
Characterizing non-Markovian quantum dynamics is essential for accurately modeling open quantum systems, particularly in near-term quantum technologies. In this work, we develop a structure-preserving approach to characterizing non-Markovian evolution using the time-convolutionless (TCL) master equation, considering both linear and nonlinear formulations. To parameterize the master equation, we explore two distinct techniques: the Karhunen-Loeve (KL) expansion, which provides an optimal basis representation of the dynamics, and neural networks, which offer a data-driven approach to learning system-environment interactions. We demonstrate our methodology using experimental data from a superconducting qubit at the Quantum Device Integration Testbed (QuDIT) at Lawrence Livermore National Laboratory (LLNL). Our results show that while neural networks can capture complex dependencies, the KL expansion yields the most accurate predictions of the qubit's non-Markovian dynamics, highlighting its effectiveness in structure-preserving quantum system characterization. These findings provide valuable insights into efficient modeling strategies for open quantum systems, with implications for quantum control and error mitigation in near-term quantum processors.
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 study the dynamics of open quantum systems driven by an external time-periodic force. Combining Floquet theory and the time-convolutionless projection operator technique we derive a time-local quantum master equation which exactly takes into account the periodic driving, while treating the system-environment interaction within second order in the coupling strength without performing the Markov approximation. The resulting equation of motion for the reduced density matrix is called Floquet time-convolutionless master equation. Employing the example of the driven spin-boson system, we demonstrate that this master equation is capable of describing strong non-Markovian effects, while yielding the Floquet-Lindblad master equation in the Markovian limit. A characteristic feature of memory effects in such driven dissipative systems is the emergence of sharp peaks of the trace-distance based non-Markovianity measure as a function of the driving amplitude, which can be traced back to quasienergy crossings leading to almost decoherence-protected subspaces through a quasienergy-induced dissipative decoupling mechanism.