87,331 research outputs found
Diffusion-Controlled Electron Transfer Processes and Power-Law Statistics of Fluorescence Intermittency of Nanoparticles
A mechanism involving diffusion-controlled electron transfer processes in Debye and non-Debye dielectric media is proposed to elucidate the power-law distribution for the lifetime of a blinking quantum dot. This model leads to two complementary regimes of power law with a sum of the exponents equal to 2, and to a specific value for the exponent in terms of a distribution of the diffusion correlation times. It also links the exponential bending tail with energetic and kinetic parameters
Determination of energetics and kinetics from single-particle intermittency and ensemble-averaged fluorescence intensity decay of quantum dots
Quantification of energetics and kinetics for the band-edge exciton states of quantum dots and the long-lived dark state is important for better understanding of the underlying mechanism for single-particle intermittency and ensemble fluorescence intensity decay. Based on a multistate diffusion-reaction model by extending our previous studies, we analyze experimental data from ensemble measurements and fluorescence intermittency of single quantum dots and determine important molecular-based quantities such as Stokes shift, free energy gap, activation energy, reorganization energy, and other kinetic parameters
Orbiting valence quarks and their influence on the structure functions of the nucleon
It is shown that intrinsic orbital motion of the valence quarks has large
influences on the spin-dependent as well as the spin-averaged nucleon structure
functions. Its connection with the observed ``very small contribution of quark
spin to nucleon spin'' and the observed violation of Gottfried sum rule is
discussed.Comment: 10 pages (LaTeX) including 3 figure
Chain dynamics and power-law distance fluctuations of single-molecule systems
Chain-dynamics-induced distance fluctuations between any two points in a finite chain with or without cross links are investigated. This model leads to three regimes of temporal behavior for distance autocorrelation: (i) initial flat time dependence, (ii) t–alpha power law, and (iii) long-time exponential decay. For an ideal Rouse chain with frequency-independent friction, alpha=(1/2). The span of the characteristic power-law behavior of a long chain could be reduced significantly with the presence of cross links
Mechanisms of fluorescence blinking in semiconductor nanocrystal quantum dots
The light-induced spectral diffusion and fluorescence intermittency (blinking) of semiconductor nanocrystal quantum dots are investigated theoretically using a diffusion-controlled electron-transfer (DCET) model, where a light-induced one-dimensional diffusion process in energy space is considered. Unlike the conventional electron-transfer reactions with simple exponential kinetics, the model naturally leads to a power-law statistics for the intermittency. We formulate a possible explanation for the spectral broadening and its proportionality to the light energy density, the –3/2 power law for the blinking statistics of the fluorescence intermittency, the breakdown of the power-law behavior with a bending tail for the "light" periods, a lack of bending tail for the "dark" periods (but would eventually appear at later times), and the dependence of the bending tail on light intensity and temperature. This DCET model predicts a critical time tc (a function of the electronic coupling strength and other quantities), such that for times shorter than tc the exponent for the power law is –1/2 instead of –3/2. Quantitative analyses are made of the experimental data on spectral diffusion and on the asymmetric blinking statistics for the "on" and "off" events. Causes for deviation of the exponent from the ideal value of –3/2 are also discussed. Several fundamental properties are determined from the present experimental data, the diffusion correlation time, the Stokes shift, and a combination of other molecular-based quantities. Specific experiments are suggested to test the model further, extract other molecular properties, and elucidate more details of the light-induced charge-transfer dynamics in quantum dots
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