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The Journal of Chemical Physics

From power law intermittence to macroscopic coherent regime

Mauro Bologna, Adrián A. Budini, Filippo Giraldi, Paolo Grigolini A

Published Jun 25, 2009• 4 citations
Publisher

Abstract

We address the problem of establishing which is the proper form of quantum master equation generating a survival probability identical to that corresponding to the nonergodic sequence of "light on" and "light off" fluorescence fluctuations in blinking quantum dots. We adopt a theoretical perspective based on the assumption that the abrupt transitions from the light on to light off state are the results of many collisions between system and environment, properly described by the Lindblad equation, and that between two consecutive collisions the system dynamics are frozen. This generates a quantum master equation belonging to the recently proposed class of generalized Lindblad equations, with a time convoluted structure, involving in the specific case of this paper both the unitary and the nonunitary contribution of the Lindblad equation. This is the property that under the low-frequency condition makes the new class of generalized Lindblad equation generates the required survival probability. We make the conjecture that this equation corresponds to the cooperative dynamics of many units that, in isolation, are described by the ordinary Lindblad equation. When the time scale of the unitary term of the Lindblad equation is shorter than the dephasing time, the cooperation generates a surprisingly extended macroscopic coherence.

DOI
10.1063/1.3156807

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We address the problem of establishing which is the proper form of quantum master equation generating a survival probability identical to that corresponding to the nonergodic sequence of "light on" and "light off" fluorescence fluctuations in blinking quantum dots. We adopt a theoretical perspective based on the assumption that the abrupt transitions from the light on to light off state are the results of many collisions between system and environment, properly described by the Lindblad equation, and that between two consecutive collisions the system dynamics are frozen. This generates a quantum master equation belonging to the recently proposed class of generalized Lindblad equations, with a time convoluted structure, involving in the specific case of this paper both the unitary and the nonunitary contribution of the Lindblad equation. This is the property that under the low-frequency condition makes the new class of generalized Lindblad equation generates the required survival probability. We make the conjecture that this equation corresponds to the cooperative dynamics of many units that, in isolation, are described by the ordinary Lindblad equation. When the time scale of the unitary term of the Lindblad equation is shorter than the dephasing time, the cooperation generates a surprisingly extended macroscopic coherence.
This thesis addresses the problem of a form of anomalous decoherence that sheds light into the spectroscopy of blinking quantum dots. The system studied is a two-state system, interacting with an external environment that has the effect of establishing an interaction between the two states, via a coherence generating coupling, called inphasing. The collisions with the environment produce also decoherence, named dephasing. Decoherence is interpreted as the entanglement of the coherent superposition of these two states with the environment. The joint action of inphasing and dephasing generates a Markov master equation statistically equivalent to a random walker jumping from one state to the other. This model can be used to describe intermittent fluorescence, as a sequence of "light on" and "light off" states. The experiments on blinking quantum dots indicate that the sojourn times are distributed with an inverse power law. Thus, a proposal to turn the model for Poisson fluorescence intermittency into a model for non-Poisson fluorescence intermittency is made. The collision-like interaction of the two-state system with the environment is assumed to takes place at random times rather than at regular times. The time distance between one collision and the next is given by a distribution, called the subordination distribution. If the subordination distribution is exponential, a sequence of collisions yielding no persistence is turned into a sequence of "light on" and "light off" states with significant persistence. If the subordination function is an inverse power law the sequel of "light on" and "light off" states becomes equivalent to the experimental sequences. Different conditions are considered, ranging from predominant inphasing to predominant dephasing. When dephasing is predominant the sequel of "light on" and "light off" states in the time asymptotic limit becomes an inverse power law. If the predominant dephasing involves a time scale much larger than the minimum time scale accessible to the experimental observation, thereby generating persistence, the resulting distribution becomes a Mittag-Leffler function. If dephasing is predominant, in addition to the inverse power law distribution of "light off" and "light on" time duration, a strong correlation between "light on" and "light off" state is predicted.
In this paper we derive an extra class of non-Markovian master equations where the system state is written as a sum of auxiliary matrixes whose evolution involve Lindblad contributions with local coupling between all of them, resembling the structure of a classical rate equation. The system dynamics may develop strong nonlocal effects such as the dependence of the stationary properties with the system initialization. These equations are derived from alternative microscopic interactions, such as complex environments described in a generalized Born-Markov approximation and tripartite system-environment interactions, where extra unobserved degrees of freedom mediates the entanglement between the system and a Markovian reservoir. Conditions that guarantee the completely positive condition of the solution map are found. Quantum stochastic processes that recover the system dynamics in average are formulated. We exemplify our results by analyzing the dynamical action of nontrivial structured dephasing and depolarizing reservoirs over a single qubit.
In this thesis a formalism for indistinguishable multi-level quantum emitters in quantum master equations is developed. The complexity of the approach scales only polynomially in the number of quantum emitters. Complexity here means the number of coupled equations or rather the dimension of the Liouville space. This approach opens new possibilities for calculating open quantum systems. The method is implemented in the PsiQuaSP library, which allows to setup and solve arbitrary master equations, in particular master equations with the reduced polyno-mial scaling. The introduced tools are utilized to study subradiance in the open Dicke model and various cQED lasers. One of the main current research goals in quantum optics and quantum information science is the generation and stabilization of quantum coherence between distinct quantum systems. These systems can for instance be photons or quantum emitters, qubits. From a theoretical stance the difficulty with these systems is that their complexity scales in general exponentially with the system size, like the number of quantum emitters. The reduced scaling of the formalism introduced in this thesis stems from the permutation symmetry of the indistinguishable emitters. The method is derived in the context of Lindblad quantum master equations. Lindblad quantum master equations for many identical multi-level systems have been used to study funda- mental quantum optical systems, such as lasing and laser like action, various phase transitions, optical bistability, cooperative resonance fluorescence, entanglement, quantum light generation, quantum to classical transitions, super- and subradiance etc. In most of these cases the single emitter, the many emitter and the weak correlation limit can be satisfactorily treated with existing techniques, such as direct integration, phase space methods or cluster expansion. However these techniques are not well suited for the few emitter case with strong correlations. The theory developed in this thesis allows to study all these systems for moderate numbers of quantum emitters and arbitrary correlation strengths, thus filling the gap left open by conventional methods. Even though the theory is developed around Lindblad quantum master equations it is not limited to this case – the requirement of indistinguishability is used to construct symmetrized Liouville space basis states and operators which can also be used to construct other master equations. In this thesis the general methodology for the polynomial scaling of the many emitter master equation is derived by two different approaches. Generalized permutation symmetric Liouville space states and operators are introduced that allow for the construction of arbitrary master equations and observables. These Liouville space states and operators are translated into a graphical representation that greatly facilitates their usage. This representation is found to have a close connection to Lie algebras as well as graph theory. The whole method is implemented in a general and modular way in a C++ library called PsiQuaSP, which allows to simulate arbitrary master equations based on a number state representation. The design of the library heavily relies on the introduced graphical representation, which greatly facilitates the setup of a simulation. The treatment of non-identical systems with PsiQuaSP is illustrated and further techniques for complexity reduction and computational speedup are discussed. These tools are applied to the two main cases of cQED lasers/spasers and super-, subradiance. In the latter case a new type of phase transition in the open Dicke model is predicted that leads to a deterministic generation of subradiant steady state coherences, with applications in quantum information science. Furthermore the interaction of quantum dots with the dissipative modes at metal interfaces is investigated in order to explain experimental findings.
The Lindblad (GKLS) master equation, which represents the mathematical form for the general evolution of a density matrix, is a versatile and widely-used tool in open quantum systems. In contrast with the typical approach of imposing additional conditions on the system, such as weak coupling or energy conservation, we explore the structure of the equation with no assumptions. We demonstrate that general quantum dynamics can be expressed through a combination of free evolution, exchanges of some physical quantities (generalised charges), not necessarily commuting with the Hamiltonian, between the system and the bath, and pure dephasing. This result comprises a novel perspective on quantum master equations, employing physical processes as elemental parts. We use it to explore the dynamics and stationary states of a two-level system and show that strong coupling, particle exchange, and non-Abelian effects all share the same physical origin. Moreover, we demonstrate that the generalised Gibbs state for all three cases contains a non-commutation term, which has not been previously considered.
The Lindblad master equation is widely used to describe the reduced dynamics of open quantum systems under Markovian assumptions. Here, we investigate its ability to reproduce the reduced evolution emerging from a microscopic many-body model in which two interacting two-level subsystems are embedded in a larger environment and evolve under fully unitary dynamics. The exact evolution exhibits a clear separation of timescales. At short times, decoherence arises from environmentally induced dephasing, leading to a Gaussian suppression of coherences and a quadratic decay of purity. At intermediate times, collective decoherence channels saturate and a slower, still Gaussian, decay driven by relative environmental fluctuations dominates. At later times the system settles in a complete decohered state. The first two behaviors cannot be reproduced by a Lindblad dynamics with constant coefficients, which always results in an exponential decay: Our work provides a simple example of the breakdown of the effective description relevant in many realistic settings.
We derive the general form of a master equation describing the reduced time evolution of a sequence of subsystems "propagating" in an environment which can be described as a sequence of subenvironments. The interaction between subsystems and subenvironments is described in terms of a collision model, with the irreversible dynamics of the subenvironments between collisions explicitly taken into account. In the weak coupling regime, we show that the collisional model produces a correlated Markovian evolution for the joint density matrix of the multipartite system. The associated Lindblad superoperator contains pairwise terms describing cross correlation between the different subsystems. Such a model can describe a broad range of physical situations, ranging from quantum channels with memory to photon propagation in concatenated quantum optical systems.