255 research outputs found
A comparison study of the Shannon channel capacity of various nonlinear optical fibers
A comparative study of the Shannon channel capacity is presented for a dispersion-free fiber, a fiber with constant dispersion, and a fiber with variable dispersion. Improvement of the capacity by optical phase conjugation (OPC) is also investigated. Simple scaling laws are prescribed for the dependence of the optimal capacity on various system settings such as number of spans, number of channels, noise power, channel width, strength of chromatic dispersion, bandwidth of an OPC device, etc
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
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
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
Distance versus energy fluctuations and electron transfer in single protein molecules
Stochastic nature due to distance and energy fluctuations of single protein molecules involved in electron-transfer (ET) reactions is studied. Distance fluctuations have been assumed previously for causing the slow fluctuations in the ET rates between a donor-acceptor pair constrained to a native protein. Although the observed t–1/2 power law can be derived using Langevin dynamics with a simple chain model, some discrepancies exist. The friction coefficient and the Rouse segment time constant deduced from experimental data are several orders of magnitude too large, even though the extracted force constant is reasonable. Therefore, questions are raised about the distance-fluctuation mechanism and the activationless ET hypothesis. As an alternative mechanism, we considered fluctuations in activation energy and analyzed the data from two different single protein experiments to determine spectral distribution of energy fluctuations
Dynamics and control of gold-encapped gallium arsenide nanowires imaged by 4D electron microscopy
Eutectic related reaction is a special chemical/physical reaction involving
multiple phases, solid and liquid. Visualization of phase reaction of composite
nanomaterials with high spatial and temporal resolution provides a key
understanding of alloy growth with important industrial applications. However,
it has been a rather challenging task. Here we report the direct imaging and
control of the phase reaction dynamics of a single, as-grown free-standing
gallium arsenide nanowire encapped with a gold nanoparticle, free from
environmental confinement or disturbance, using four-dimensional electron
microscopy. The non-destructive preparation of as-grown free-standing nanowires
without supporting films allows us to study their anisotropic properties in
their native environment with better statistical character. A laser heating
pulse initiates the eutectic related reaction at a temperature much lower than
the melting points of the composite materials, followed by a precisely
time-delayed electron pulse to visualize the irreversible transient states of
nucleation, growth and solidification of the complex. Combined with theoretical
modeling, useful thermodynamic parameters of the newly formed alloy phases and
their crystal structures could be determined. This technique of dynamical
control and 4D imaging of phase reaction processes on the nanometer-ultrafast
time scale open new venues for engineering various reactions in a wide variety
of other systems
Plasma-induced unconventional shock waves on oil surfaces
Electric corona discharge in a multi-phase system results in complex electro-hydrodynamic phenomena. We observed unconventional shock wave propagation on an oil thin film sprayed over a polymer-coated conductor. A hair-thin single shock wave arose when the high voltage bias of an overhung steel needle was abruptly removed. However, such solitary waves possess neither interference nor reflection properties commonly known for ordinary waves, and also differ from the solitons in a canal or an optical fiber. We also observed time-retarded movement for dispersed oil droplets at various distances from the epicenter which have no physical contact, as if a wave propagating on a continuous medium. Such a causality phenomenon for noncontact droplets to move resembling wave propagation could not be possibly described by the conventional surface wave equation. Our systematic studies reveal a mechanism involving oil surface charges driven by reminiscent electric fields in the air when the needle bias is suddenly removed
Imaging rotational dynamics of nanoparticles in liquid by 4D electron microscopy
In real time and space, four-dimensional electron microscopy (4D EM) has enabled observation of transient structures and morphologies of inorganic and organic materials. We have extended 4D EM to include liquid cells without the time resolution being limited by the response of the detector. Our approach permits the imaging of the motion and morphological dynamics of a single, same particle on nanometer and ultrashort time scales. As a first application, we studied the rotational dynamics of gold nanoparticles in aqueous solution. A full transition from the conventional diffusive rotation to superdiffusive rotation and further to a ballistic rotation was observed with increasing asymmetry of the nanoparticle morphology. We explored the underlying physics both experimentally and theoretically according to the morphological asymmetry of the nanoparticles
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