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arXiv:0711.0074 · Journal of Physics A Mathematical and Theoretical

Staying positive: going beyond Lindblad with perturbative master equations

Robert S. Whitney

Published Apr 15, 2008• 107 citations
arXivHTMLPDF

Abstract

The perturbative master equation (Bloch–Redfield) is used extensively to study dissipative quantum mechanics—particularly for qubits—despite the 25-year-old criticism that it violates positivity (generating negative probabilities). We take an arbitrary system coupled to an environment containing many degrees-of-freedom and cast its perturbative master equation (derived from a perturbative treatment of Nakajima–Zwanzig or Schoeller–Schön equations) in the form of a Lindblad master equation. We find that the equation's parameters are time dependent . This time dependence is rarely accounted for and invalidates Lindblad's dynamical semigroup analysis. We analyse one such Bloch–Redfield master equation (for a two-level system coupled to an environment with a short but non-vanishing memory time), which apparently violates positivity. We analytically show that, once the time dependence of the parameters is accounted for, positivity is preserved.

DOI
10.1088/1751-8113/41/17/175304

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The perturbative master equation (Bloch–Redfield) is used extensively to study dissipative quantum mechanics—particularly for qubits—despite the 25-year-old criticism that it violates positivity (generating negative probabilities). We take an arbitrary system coupled to an environment containing many degrees-of-freedom and cast its perturbative master equation (derived from a perturbative treatment of Nakajima–Zwanzig or Schoeller–Schön equations) in the form of a Lindblad master equation. We find that the equation's parameters are time dependent . This time dependence is rarely accounted for and invalidates Lindblad's dynamical semigroup analysis. We analyse one such Bloch–Redfield master equation (for a two-level system coupled to an environment with a short but non-vanishing memory time), which apparently violates positivity. We analytically show that, once the time dependence of the parameters is accounted for, positivity is preserved.
Master equations play a pivotal role in investigating open quantum systems. In particular, the Bloch-Redfield equation stands out due to its relation to a concrete physical environment. However, without further approximations it does not lead to a Lindblad master equation that guarantees that the density matrix stays completely positive, which has raised some concerns regarding its use. This study builds on previous efforts to transform the Bloch-Redfield framework into a mathematically robust Lindblad equation while fully preserving the effects that are lost within the secular approximation that is commonly used to guarantee positivity. These previous approaches introduced two potential deficiencies: The environment-induced energy shift can be non-Hermitian and some decay rates can be negative, violating the assumptions of Lindblad's theorem. Here we propose and evaluate straightforward solutions to both problems. Our approach offers an effective and general procedure for obtaining a Lindblad equation, derived from a concrete physical environment, while mitigating the unphysical dynamics present in the Bloch-Redfield equation.
The reduced dynamics of an open quantum system obtained from an underlying microscopic Hamiltonian can in general only approximately be described by a time-local master equation. The quality of that approximation depends primarily on the coupling strength and the structure of the environment. Various such master equations have been proposed with different aims. Choosing the most suitable one for a specific system is not straightforward. By focusing on the accuracy of the reduced dynamics we provide a thorough assessment for a selection of methods (Redfield equation, quantum optical master equation, coarse-grained master equation, a related dynamical map approach, and a partial-secular approximation). We consider secondary, here, whether or not an approach guarantees positivity. We use two qubits coupled to a Lorentzian environment in a spin-boson-like fashion modeling a generic situation with various system and bath time scales. We see that, independent of the initial state, the simple Redfield equation with time-dependent coefficients is significantly more accurate than all other methods under consideration. We emphasize that positivity violation in the Redfield equation formalism becomes relevant only in a regime where any of the perturbative master equations considered here are rendered invalid anyway. This implies that the loss of positivity should in fact be welcomed as an important feature: it indicates the breakdown of the weak-coupling assumption. In addition we present the various approaches in a self-contained way and use the behavior of their errors to provide further insight into the range of validity of each method.
We consider open quantum systems with dynamics described by master equations that have perturbative expansions in the system-environment interaction. We show that, contrary to intuition, full-time solutions of order-2n accuracy require an order-(2n+2) master equation. We give two examples of such inaccuracies in the solutions to an order-2n master equation: order-2n inaccuracies in the steady state of the system and order-2n positivity violations. We show how these arise in a specific example for which exact solutions are available. This result has a wide-ranging impact on the validity of coupling (or friction) sensitive results derived from second-order convolutionless, Nakajima-Zwanzig, Redfield, and Born-Markov master equations.
Data of the numerical solution of the time-dependent Schrödinger equation of a system containing one spin-1/2 particle interacting with a bath of up to 32 spin-1/2 particles is used to construct a Markovian quantum master equation describing the dynamics of the system spin. The procedure of obtaining this quantum master equation, which takes the form of a Bloch equation with time-independent coefficients, accounts for all non-Markovian effects inasmuch the general structure of the quantum master equation allows. Our simulation results show that, with a few rather exotic exceptions, the Bloch-type equation with time-independent coefficients provides a simple and accurate description of the dynamics of a spin-1/2 particle in contact with a thermal bath. A calculation of the coefficients that appear in the Redfield master equation in the Markovian limit shows that this perturbatively derived equation quantitatively differs from the numerically estimated Markovian master equation, the results of which agree very well with the solution of the time-dependent Schrödinger equation.
It is very common in the literature to write a Markovian quantum master equation in Lindblad form to describe a system with multiple degrees of freedom and weakly connected to multiple thermal baths which can, in general, be at different temperatures and chemical potentials. However, the microscopically derived quantum master equation up to leading order in a system-bath coupling is of the so-called Redfield form, which is known to not preserve complete positivity in most cases. Additional approximations to the Redfield equation are required to obtain a Lindblad form. We lay down some fundamental requirements for any further approximations to the Redfield equation, which, if violated, leads to physical inconsistencies such as inaccuracies in the leading order populations and coherences in the energy eigenbasis, violation of thermalization, and violation of local conservation laws at the nonequilibrium steady state. We argue that one or more of these conditions will generically be violated in all the weak system-bath-coupling Lindblad descriptions existing in the literature to our knowledge. As an example, we study the recently derived universal Lindblad equation and use these conditions to show the violation of local conservation laws due to inaccurate coherences but accurate populations in the energy eigenbasis. Finally, we exemplify our analytical results numerically in an interacting open quantum spin system.
Positivity preservation is naturally guaranteed in exact non-Markovian master equations for open quantum system dynamics. However, in many approximated non-Markovian master equations, the positivity of the reduced density matrix is not guaranteed. In this paper we provide a general class of time-local, perturbative, and positivity-preserving non-Markovian master equations generated from stochastic Schr\"odinger equations, particularly quantum-state-diffusion equations. Our method has an expanded range of applicability for accommodating a variety of non-Markovian environments. We show the positivity-preserving master equation for a three-level system coupled to a dissipative bosonic environment as a particular example to exemplify our general approach. We illustrate the numerical simulations with an analysis explaining why the previous approximated non-Markovian master equations cannot guarantee positivity. Our work provides a consistent master equation for studying the non-Markovian dynamics in ultrafast quantum processes and strong-coupling systems.