Statistical Aging and Nonergodicity in the Fluorescence of Single Nanocrystals

Brokmann, Xavier; Hermier, Jean-Pierre; Messin, Gaëtan; Desbiolles, Pierre; Bouchaud, Jean‐Philippe; Dahan, Maxime

doi:10.1103/physrevlett.90.120601

Cited by 381 publications

(409 citation statements)

References 27 publications

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“…periods and remain dark during others [63][64][65]. The durations of these on periods and off periods are found to be distributed according to a power law whose exponent is such that the average on and off time is infinite (i.e., of the order of the measurement time), leading to aging in the intensity autocorrelation function [7,66]. This model is the familiar Lévy walk [12,31,36,67], which is a popular stochastic framework with many applications.…”

Section: Blinking Quantum Dots and Lévy Walkmentioning

confidence: 99%

Scaling Green-Kubo Relation and Application to Three Aging Systems

et al. 2014

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The Green-Kubo formula relates the spatial diffusion coefficient to the stationary velocity autocorrelation function. We derive a generalization of the Green-Kubo formula that is valid for systems with longrange or nonstationary correlations for which the standard approach is no longer valid. For the systems under consideration, the velocity autocorrelation function hvðt þ τÞvðtÞi asymptotically exhibits a certain scaling behavior and the diffusion is anomalous, hx 2 ðtÞi ≃ 2D ν t ν . We show how both the anomalous diffusion coefficient D ν and the exponent ν can be extracted from this scaling form. Our scaling GreenKubo relation thus extends an important relation between transport properties and correlation functions to generic systems with scale-invariant dynamics. This includes stationary systems with slowly decaying power-law correlations, as well as aging systems, systems whose properties depend on the age of the system. Even for systems that are stationary in the long-time limit, we find that the long-time diffusive behavior can strongly depend on the initial preparation of the system. In these cases, the diffusivity D ν is not unique, and we determine its values, respectively, for a stationary or nonstationary initial state. We discuss three applications of the scaling Green-Kubo relation: free diffusion with nonlinear friction corresponding to cold atoms diffusing in optical lattices, the fractional Langevin equation with external noise recently suggested to model active transport in cells, and the Lévy walk with numerous applications, in particular, blinking quantum dots. These examples underline the wide applicability of our approach, which is able to treat very different mechanisms of anomalous diffusion.

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Section: Blinking Quantum Dots and Lévy Walkmentioning

confidence: 99%

Scaling Green-Kubo Relation and Application to Three Aging Systems

et al. 2014

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“…It is worth 035303-3 noting that for CdSe/ZnS NCs the ACF also depends strongly on the considered time interval for the calculation. All these properties were related to the power-law statistics followed by the duration of the extinction periods 34 that is not observed for CdSe/CdS NCs. 2,35 Even if the ACF remains close to 1, the slight deviation from unity has a strong impact in terms of intensity fluctuations.…”

Section: Intensity Fluctuationsmentioning

confidence: 99%

Blinking suppression and biexcitonic emission in thick-shell CdSe/CdS nanocrystals at cryogenic temperature

et al. 2014

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The fluorescence of single colloidal thick-shell CdSe/CdS nanocrystals (NCs), at cryogenic temperature (4 K) and room temperature (RT), is studied using the intensity autocorrelation function (ACF) and lifetime measurements. The radiative and Auger decay rates corresponding to the desexcitation of the charged biexcitonic state are determined through an original method of photon postselection. Especially, the charged biexciton quantum yield increases from about 15% at RT to 60% at 4 K. The high inhibition of Auger recombination already observed for the trion state of CdSe/CdS NCs at low temperature is also demonstrated for the charged biexcitonic state. At 4 K, the ACF is equal to 1 for time scales ranging from 50 ns to 200 ms. In contrast with RT operation, the intensity of the trion emission is then perfectly stable and no blinking is observed. All the results highlight the strong confinement of the charge carriers in the CdSe core.

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“…According to a widely shared theoretical interdisciplinary perspective, ranging from neurophysiology to sociology, from geophysics to economics, heavy tails and inverse power law distributions [2,3] are thought to be the signature of complexity. Of special interest are the scale-free distributions in time, for instance, the waiting time distributions of the "light on" and "light off" states of intermittent fluorescence in quantum dots [4][5][6][7], which has been proved [8,9] to be a renewal non-Poisson process. These scale-free waiting time distribution densities have the time-asymptotic form…”

Section: Introductionmentioning

confidence: 99%

Cooperation in neural systems: Bridging complexity and periodicity

Zare

Grigolini

2012

Phys. Rev. E

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Inverse power law distributions are generally interpreted as a manifestation of complexity, and waiting time distributions with power index μ < 2 reflect the occurrence of ergodicity-breaking renewal events. In this paper we show how to combine these properties with the apparently foreign clocklike nature of biological processes. We use a two-dimensional regular network of leaky integrate-and-fire neurons, each of which is linked to its four nearest neighbors, to show that both complexity and periodicity are generated by locality breakdown: Links of increasing strength have the effect of turning local interactions into long-range interactions, thereby generating time complexity followed by time periodicity. Increasing the density of neuron firings reduces the influence of periodicity, thus creating a cooperation-induced renewal condition that is distinctly non-Poissonian.

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Statistical Aging and Nonergodicity in the Fluorescence of Single Nanocrystals

Cited by 381 publications

References 27 publications

Scaling Green-Kubo Relation and Application to Three Aging Systems

Scaling Green-Kubo Relation and Application to Three Aging Systems

Blinking suppression and biexcitonic emission in thick-shell CdSe/CdS nanocrystals at cryogenic temperature

Cooperation in neural systems: Bridging complexity and periodicity

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