Subnanosecond spectral diffusion measurement using photon correlation

Spectral diffusion is a result of random spectral jumps of a narrow line as a result of a fluctuating environment. It is an important issue in spectroscopy, because the observed spectral broadening prevents access to the intrinsic line properties. However, its characteristic parameters provide local information on the environment of a light emitter embedded in a solid matrix, or moving within a fluid, leading to numerous applications in physics and biology. We present a new experimental technique for measuring spectral diffusion based on photon correlations within a spectral line. Autocorrelation on half of the line and cross-correlation between the two halves give a quantitative value of the spectral diffusion time, with a resolution only limited by the correlation set-up. We have measured spectral diffusion of the photoluminescence of a single light emitter with a time resolution of 90 ps, exceeding by four orders of magnitude the best resolution reported to date

Generalized Arcsine Law and Stable Law in an Infinite Measure Dynamical System

Limit theorems for the time average of some observation functions in an infinite measure dynamical system are studied. It is known that intermittent phenomena, such as the Rayleigh-Benard convection and Belousov-Zhabotinsky reaction, are described by infinite measure dynamical systems.We show that the time average of the observation function which is not the $L^1(m)$ function, whose average with respect to the invariant measure $m$ is finite, converges to the generalized arcsine distribution. This result leads to the novel view that the correlation function is intrinsically random and does not decay. Moreover, it is also numerically shown that the time average of the observation function converges to the stable distribution when the observation function has the infinite mean.Comment: 8 pages, 8 figure

Energy Transfer from Individual Semiconductor Nanocrystals to Graphene

Energy transfer from photoexcited zero-dimensional systems to metallic systems plays a prominent role in modern day materials science. A situation of particular interest concerns the interaction between a photoexcited dipole and an atomically thin metal. The recent discovery of graphene layers permits investigation of this phenomenon. Here we report a study of fluorescence from individual CdSe/ZnS nanocrystals in contact with single- and few-layer graphene sheets. The rate of energy transfer is determined from the strong quenching of the nanocrystal fluorescence. For single-layer graphene, we find a rate of ~ 4ns-1, in agreement with a model based on the dipole approximation and a tight-binding description of graphene. This rate increases significantly with the number of graphene layers, before approaching the bulk limit. Our study quantifies energy transfer to and fluorescence quenching by graphene, critical properties for novel applications in photovoltaic devices and as a molecular ruler

Statistical Aging and Non Ergodicity in the Fluorescence of Single Nanocrystals

The relation between single particle and ensemble measurements is adressed for semiconductor CdSe nanocrystals. We record their fluorescence at the single molecule level and analyse their emission intermittency, which is governed by unusual random processes known as Levy statistics. We report the observation of statistical aging and ergodicity breaking, both related to the occurrence of Levy statistics. Our results show that the behaviour of ensemble quantities, such as the total fluorescence of an ensemble of nanocrystals, can differ from the time averaged individual quantities, and must be interpreted with care.Comment: 4 pages, 3 figure

Weakly non-ergodic Statistical Physics

We find a general formula for the distribution of time averaged observables for weakly non-ergodic systems. Such type of ergodicity breaking is known to describe certain systems which exhibit anomalous fluctuations, e.g. blinking quantum dots and the sub-diffusive continuous time random walk model. When the fluctuations become normal we recover usual ergodic statistical mechanics. Examples of a particle undergoing fractional dynamics in a binding force field are worked out in detail. We briefly discuss possible physical applications in single particle experiments

Sample-Averaged Biexciton Quantum Yield Measured by Solution-Phase Photon Correlation

The brightness of nanoscale optical materials such as semiconductor nanocrystals is currently limited in high excitation flux applications by inefficient multiexciton fluorescence. We have devised a solution-phase photon correlation measurement that can conveniently and reliably measure the average biexciton-to-exciton quantum yield ratio of an entire sample without user selection bias. This technique can be used to investigate the multiexciton recombination dynamics of a broad scope of synthetically underdeveloped materials, including those with low exciton quantum yields and poor fluorescence stability. Here, we have applied this method to measure weak biexciton fluorescence in samples of visible-emitting InP/ZnS and InAs/ZnS core/shell nanocrystals, and to demonstrate that a rapid CdS shell growth procedure can markedly increase the biexciton fluorescence of CdSe nanocrystals.United States. Dept. of Energy. Office of Basic Energy Sciences (DE-FG02-07ER46454)United States. Dept. of Energy. Office of Basic Energy Sciences (DE-SC0001088)National Institutes of Health (U.S.) (9P41EB015871-26A1

Quantum regression theorem for non-Markovian Lindblad equations

We find the conditions under which a quantum regression theorem can be assumed valid for non-Markovian master equations consisting in Lindblad superoperators with memory kernels. Our considerations are based on a generalized Born-Markov approximation, which allows us to obtain our results from an underlying Hamiltonian description. We demonstrate that a non-Markovian quantum regression theorem can only be granted in a stationary regime if the dynamics satisfies a quantum detailed balance condition. As an example we study the correlations of a two level system embedded in a complex structured reservoir and driven by an external coherent field.Comment: 14 pages, 5 figures. Extended version. The GBMA is deduced from projector technique. A new appendix is adde

Probing and controlling fluorescence blinking of single semiconductor nanoparticles

In this review we present an overview of the experimental and theoretical development on fluorescence intermittency (blinking) and the roles of electron transfer in semiconductor crystalline nanoparticles. Blinking is a very interesting phenomenon commonly observed in single molecule/particle experiments. Under continuous laser illumination, the fluorescence time trace of these single nanoparticles exhibit random light and dark periods. Since its first observation in the mid-1990s, this intriguing phenomenon has attracted wide attention among researchers from many disciplines. We will first present the historical background of the discovery and the observation of unusual inverse power-law dependence for the waiting time distributions of light and dark periods. Then, we will describe our theoretical modeling efforts to elucidate the causes for the power-law behavior, to probe the roles of electron transfer in blinking, and eventually to control blinking and to achieve complete suppression of the blinking, which is an annoying feature in many applications of quantum dots as light sources and fluorescence labels for biomedical imaging