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Physical review. B, Condensed matter

Effect of trapping on transport coherence. II. Continuous-time random-walk treatment

Pavel Heřman, Ivan Barvı́k

Published Aug 1, 1993• 6 citations
Publisher

Abstract

Our recent investigation led to the conclusion that there is much agreement among theories of the excitation transfer: the generalized master equation (GME), the Haken-Strobl-Reineker stochastic-Liouville-equation theory, and the Grover-Silbey microscopic theory. Trapping effects influence memory functions entering the GME. Decoupling of the rest of the system from the sink in the nearly coherent regime for large trapping rates changes the form of the pausing-time-distribution functions and probability densities in the continuous-time random-walk method.

DOI
10.1103/physrevb.48.3130

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Our recent investigation led to the conclusion that there is much agreement among theories of the excitation transfer: the generalized master equation (GME), the Haken-Strobl-Reineker stochastic-Liouville-equation theory, and the Grover-Silbey microscopic theory. Trapping effects influence memory functions entering the GME. Decoupling of the rest of the system from the sink in the nearly coherent regime for large trapping rates changes the form of the pausing-time-distribution functions and probability densities in the continuous-time random-walk method.
It is shown in this paper that the quantum master equation can be mapped to a modified continuous time random walk (CTRW) if the relaxation term is composed of transitions over a set of states. When the Hamiltonian is time-independent and transitions are between its eigenlevels, such a modified CTRW reduces to the Markovian walk equivalent to the Pauli master equation. On the other hand, the memory in such a modified CTRW is composed of a temporal factor and the probability determined by the Liouville flow when the relaxation term is reduced as a special dephasing term.
Recent findings suggest that processes such as the excitonic energy transfer through the photosynthetic antenna display quantal features, aspects known from the dynamics of charge carriers along polymer backbones. Hence, in modeling energy transfer one has to leave the classical, master-equation-type formalism and advance towards an increasingly quantum-mechanical picture, while still retaining a local description of the complex network of molecules involved in the transport, say through a tight-binding approach. Interestingly, the continuous time random walk (CTRW) picture, widely employed in describing transport in random environments, can be mathematically reformulated to yield a quantum-mechanical Hamiltonian of tight-binding type; the procedure uses the mathematical analogies between time-evolution operators in statistical and in quantum mechanics: The result are continuous-time quantum walks (CTQWs). However, beyond these formal analogies, CTRWs and CTQWs display vastly different physical properties. In particular, here we focus on trapping processes on a ring and show, both analytically and numerically, that distinct configurations of traps (ranging from periodical to random) yield strongly different behaviors for the quantal mean survival probability, while classically (under ordered conditions) we always find an exponential decay at long times.
Most traditional discussions of the Markoffian Born approximation of relaxation phenomena (e.g., Bloch equations) are based on the assumption of widely separated time scales in the non-Markoffian weak coupling generalized master equation. By exploiting the physically reasonable Gaussian factorization property of multitime correlation functions which enter through the system reservoir interaction, recent work has shed significant new light on the relationship between the Markoffian-Born approximation and the exact generalized master equation (GME) describing the evolution of the relaxing subsystem. Two limits for which the GME becomes the Born approximation relaxation equation arc discussed: (1) the Van Hove (λ2t) limit rigorously discussed for open systems by Davies, (2) the zero memory (white noise) suggested by Middleton—Schieve and recently discussed for open systems by Gorini—Kossakawsky and Palmer. We have outlined the proof of this limit. We then discuss the physical meaning of these two exact limits in the context of the general theory of kinetic equations of Resibois. The dominant pole contributions are isolated to all orders by means of an expansion in which the terms are in norm proportional to powers of the ratio of the time scales τc/τB where τc is the two point correlation memory time and τB the relaxation time in the Born approximation. Each of the above exact limits corresponds to the vanishing of this ratio. Comments are made on nonexponential decay.
Recent findings suggest that processes such as the electronic energy transfer through the photosynthetic antenna display quantal features, aspects known from the dynamics of charge carriers along polymer backbones. Hence, in modeling energy transfer one has to leave the classical, masterequation-type formalism and advance towards an increasingly quantum-mechanical picture, while still retaining a local description of the complex network of molecules involved in the transport, say through a tight-binding approach. Interestingly, the continuous time random walk (CTRW) picture, widely employed in describing transport in random environments, can be mathematically reformulated to yield a quantummechanical Hamiltonian of tight-binding type; the procedure uses the mathematical analogies between time-evolution operators in statistical and in quantum mechanics: The result are continuoustime quantum walks (CTQWs). However, beyond these formal analogies, CTRWs and CTQWs display vastly different physical properties. In particular, here we focus on trapping processes on a ring and show, both analytically and numerically, that distinct configurations of traps (ranging from periodical to random) yield strongly different behaviours for the quantal mean survival probability, while classically (under ordered conditions) we always find an exponential decay at long times.
Stochastic treatments of magnetic resonance spectroscopy and optical spectroscopy require evaluations of functions such as (exp(i ∫(0)(t) Q(s)ds)), where t is time, Q(s) is the value of a stochastic process at time s, and the angular brackets denote ensemble averaging. This paper gives an exact evaluation of these functions for the case where Q is a continuous-time random walk process. The continuous-time random walk describes an environment that undergoes slow steplike changes in time. It also has a well-defined Gaussian limit and so allows for non-Gaussian and Gaussian stochastic dynamics to be studied within a single framework. We apply the results to extract qubit-lattice interaction parameters from dephasing data of P-doped Si semiconductors (data collected elsewhere) and to calculate the two-dimensional spectrum of a three-level harmonic oscillator undergoing random frequency modulations.
We introduce the quantum Lévy walk to study transport and decoherence in a quantum random model. We have derived from second-order perturbation theory the quantum master equation for a Lévy-like particle that moves along a lattice through scale-free hopping while interacting with a thermal bath of oscillators. The general evolution of the quantum Lévy particle has been solved for different preparations of the system. We examine the evolution of the quantum purity, the localized correlation and the probability to be in a lattice site, all of them leading to important conclusions concerning quantum irreversibility and decoherence features. We prove that the quantum thermal mean-square displacement is finite under a constraint that is different when compared to the classical Weierstrass random walk. We prove that when the mean-square displacement is infinite the density of state has a complex null-set inside the Brillouin zone. We show the existence of a critical behavior in the continuous eigenenergy which is related to its non-differentiability and self-affine characteristics. In general, our approach allows us to study analytically quantum fluctuations and decoherence in a long-range hopping model.