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Journal of Physics B Atomic Molecular and Optical Physics

Quantum jumps in non-Markovian single fluorescent systems

Adrián A. Budini

Published Jun 20, 2007• 11 citations
Publisher

Abstract

In this paper, we formulate a quantum jump approach associated with single fluorescent systems whose radiative decay is defined by a Lindblad-like equation with a memory kernel. We base our results in a generalized Born–Markov approximation, which allows us to get our results from a full microscopic description. In the weak-laser-excitation regime, the photon-emission process can be described through a delay function, which in a natural way provides the basis for unravelling the dynamics in terms of a stochastic density matrix. As in the Markovian case, the stochastic dynamics consists in periods where the evolution is smooth and non-unitary, interrupted at random times where the photon-detection events produce a sudden change in the system state. The phenomenon of non-Poissonian intermittent fluorescence induced by complex environments (Budini 2006 Phys. Rev. A 73 061802) is analysed in the context of this approach.

DOI
10.1088/0953-4075/40/13/012

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In this paper, we formulate a quantum jump approach associated with single fluorescent systems whose radiative decay is defined by a Lindblad-like equation with a memory kernel. We base our results in a generalized Born–Markov approximation, which allows us to get our results from a full microscopic description. In the weak-laser-excitation regime, the photon-emission process can be described through a delay function, which in a natural way provides the basis for unravelling the dynamics in terms of a stochastic density matrix. As in the Markovian case, the stochastic dynamics consists in periods where the evolution is smooth and non-unitary, interrupted at random times where the photon-detection events produce a sudden change in the system state. The phenomenon of non-Poissonian intermittent fluorescence induced by complex environments (Budini 2006 Phys. Rev. A 73 061802) is analysed in the context of this approach.
In this paper, we develop a quantum-jump approach for describing the photon emission process of single fluorophore systems coupled to complex classically fluctuating reservoirs. The formalism relies on an open quantum system approach where the dynamics of the system and the reservoir fluctuations are described through a density matrix whose evolution is defined by a Lindblad rate equation. For each realization of the photon-measurement processes it is possible to define a conditional system state (stochastic density matrix) whose evolution depends on both the photon detection events and the fluctuations between the configurational states of the reservoir. In contrast to standard fluorescent systems the photon-to-photon emission process is not a renewal one, being defined by a (stochastic) waiting time distribution that in each recording event parametrically depends on the conditional state. The formalism allows calculating experimental observables such as the full hierarchy of joint probabilities associated with the time intervals between consecutive photon recording events. These results provide a powerful basis for characterizing different situations arising in single-molecule spectroscopy, such as spectral fluctuations, lifetime fluctuations and light-assisted processes.
We characterize the photon-counting statistics of single-chromophore systems submitted to continuous laser radiation and embedded in a complex structured environment able to induce strong non-Markovian effects in the decay dynamics. In the weak-laser-excitation regime, the photon-emission process can be described through a delay function. We demonstrate that the dynamics, by itself, is able to develop a non-Poissonian intermittent fluorescence phenomenon where the bright and dark intervals are characterized by probability distributions that may depart from an exponential one.
Stochastic unravelings provide a useful way to represent open quantum system dynamics in terms of pure state realizations, and have been widely studied both from a fundamental and from a computational point of view. They were initially formulated for Markovian dynamics described by the Gorini-Kossakowski-Sudarshan-Lindblad master equation. However, due to recent technological and experimental development, most physical relevant dynamics present temporal correlations beyond the Markov approximation. Such correlations cause decay rates to turn temporarily negative, thus requiring the generalization of stochastic unravelings from Markovian to non-Markovian scenarios. Indeed, many unraveling techniques have been introduced in this regime, and a comprehensive review of the different jump methods is currently missing. In this work, we provide an overview of widely used quantum jump unraveling techniques for non-Markovian systems and also discuss them in terms of their numerical efficiency, divisibility requirements, Hilbert space extension, and measurement interpretation.
By considering single chromophore systems whose radiative decay can be written in terms of a nonlocal Lindblad-type evolution, the authors extend the formalism of generalized optical Bloch equations [Y. Zheng and F. L. H. Brown, Phys. Rev. Lett. 90, 238305 (2003)] to non-Markovian dynamics. They demonstrate that photon statistical properties such as bunching and antibunching, as well as sub- and super-Poissonian photon statistics can be fitted in the context of non-Markovian dynamics. The nonlocal effects may arise due to the interaction with a complex structured environment. In this case, the photon statistics can be related with the parameters that define the microscopic system-environment interaction. Alternatively, the authors demonstrate that effective dynamics such as triplet blinking, where the system is coupled via incoherent transitions to an extra dark state, can also be worked out in terms of generalized non-Markovian optical Bloch equations. The corresponding memory contributions are mapped with those that arise from the microscopic approach.
We discuss in detail how non-Markovian open system dynamics can be described in terms of quantum jumps [J. Piilo et al., Phys. Rev. Lett. 100, 180402 (2008)]. Our results demonstrate that it is possible to have a jump description contained in the physical Hilbert space of the reduced system. The developed non-Markovian quantum jump approach is a generalization of the Markovian Monte Carlo wave function (MCWF) method into the non-Markovian regime. The method conserves both the probabilities in the density matrix and the norms of the state vectors exactly and sheds new light on non-Markovian dynamics. The dynamics of the pure state ensemble illustrates how local-in-time master equation can describe memory effects and how the current state of the system carries information on its earlier state. Our approach solves the problem of negative jump probabilities of the Markovian MCWF method in the non-Markovian regime by defining the corresponding jump process with positive probability. The results demonstrate that in the theoretical description of non-Markovian open systems, there occurs quantum jumps which recreate seemingly lost superpositions due to the memory.
Strong laser fields, when tuned on resonance to an atomic (molecular) transition, give rise to the well-known triplet of resonance fluorescence. The laser field is normally assumed to be strong and monochromatic, even though the spectrum of real lasers is never a \ensuremath{\delta} function. A standard way to treat laser fluctuations has been to assume a well-defined nominal frequency and a randomly fluctuating phase. Recently we introduced the generalized jump model (GJM) for correlated phase fluctuations, where correlated phase jumps are considered, leading to Markovian as well as non-Markovian stochastic behavior. In the GJM, each phase jump may be correlated to the previous jump, and the degree of correlation, the typical jump size, and the mean time between jumps are the three parameters defining the stochastic character of the laser field. In this paper we apply the GJM model to the case of resonance fluorescence from an atom excited by a stochastic field. The ``standard'' Mollow triplet is obtained in the monochromatic limit of small jumps, and several new predictions are made in the different limits of the stochastic parameters. In the small-jump limit, a new ``field effect'' is predicted. The spectral line shape and the triplet separation deviate from the Mollow predictions for a monochromatic field in a substantial way, giving rise to observable differences.In the highly correlated small-jump limit, which is approximated by the Kubo oscillator model, the previous results are corrected to include nonzero line shifts and extended to the case of non-Lorentzian line shapes. In all regions, even input fields of the same line shape (which would be considered identical in the one-parameter linewidth description) give rise to very different output spectra, justifying the more complete stochastic description. Effective relaxation constants ${\mathrm{\ensuremath{\Gamma}}}_{1}^{\mathrm{*}}$ and ${\mathrm{\ensuremath{\Gamma}}}_{2}^{\mathrm{*}}$ that simplify the description of the spectrum are calculated in all appropriate cases, and ${\mathrm{\ensuremath{\Gamma}}}_{1}^{\mathrm{*}}$ is found to equal the input laser linewidth. In addition to predicting the resonance fluorescence spectra, the present analysis provides a way to extract the stochastic parameters from the nonlinear measurement in those cases where the linear characterization of the input field cannot do it. The analytic work is fully supported by extensive numerical simulations.