Stationary-state electronic distribution in quantum dots

We wish to draw an attention to a non-gibbsian behavior of zero-dimensional semiconductor nanostructures, which appears to be manifested in experiments by an effect of incomplete depopulation from electronic excited states or by an effect of up-conversion of electronic level occupation after preparing the system in the ground state of electronic excitation. In the present work the effect is interpreted with help of electron-LO-phonon interaction, which is supposed to play a role in these structures in the form of multiple-scattering of electron on the optical phonons. Quantum kinetic equation describing the process of electronic ralaxation with the inclusion of electronic multiple scattering on phonons is considered. The multiple electron scattering interpretation of the effect is supported by pointing out a considerable degree of agreement between the theoretical picture presented and a rather extensive amount of existing experimental data.Comment: 8 pages, 3 figure

Exploration of the memory effect on the photon-assisted tunneling via a single quantum dot: A generalized Floquet theoretical approach

The generalized Floquet approach is developed to study memory effect on electron transport phenomena through a periodically driven single quantum dot in an electrode-multi-level dot-electrode nanoscale quantum device. The memory effect is treated using a multi-function Lorentzian spectral density (LSD) model that mimics the spectral density of each electrode in terms of multiple Lorentzian functions. For the symmetric single-function LSD model involving a single-level dot, the underlying single-particle propagator is shown to be related to a 2 x 2 effective time-dependent Hamiltonian that includes both the periodic external field and the electrode memory effect. By invoking the generalized Van Vleck (GVV) nearly degenerate perturbation theory, an analytical Tien-Gordon-like expression is derived for arbitrary order multi- photon resonance d.c. tunneling current. Numerically converged simulations and the GVV analytical results are in good agreement, revealing the origin of multi- photon coherent destruction of tunneling and accounting for the suppression of the staircase jumps of d.c. current due to the memory effect. Specially, a novel blockade phenomenon is observed, showing distinctive oscillations in the field-induced current in the large bias voltage limit

Ultrafast optical generation of coherent phonons in CdTe1-xSex quantum dots

We report on the impulsive generation of coherent optical phonons in CdTe0.68Se0.32 nanocrystallites embedded in a glass matrix. Pump probe experiments using femtosecond laser pulses were performed by tuning the laser central energy to resonate with the absorption edge of the nanocrystals. We identify two longitudinal optical phonons, one longitudinal acoustic phonon and a fourth mode of a mixed longitudinal-transverse nature. The amplitude of the optical phonons as a function of the laser central energy exhibits a resonance that is well described by a model based on impulsive stimulated Raman scattering. The phases of the coherent phonons reveal coupling between different modes. At low power density excitations, the frequency of the optical coherent phonons deviates from values obtained from spontaneous Raman scattering. This behavior is ascribed to the presence of electronic impurity states which modify the nanocrystal dielectric function and, thereby, the frequency of the infrared-active phonons

Spectral densities and partition functions of modular quantum systems as derived from a central limit theorem

Using a central limit theorem for arrays of interacting quantum systems, we give analytical expressions for the density of states and the partition function at finite temperature of such a system, which are valid in the limit of infinite number of subsystems. Even for only small numbers of subsystems we find good accordance with some known, exact results.Comment: 6 pages, 4 figures, some steps added to derivation, accepted for publication in J. Stat. Phy

Evidence for a diffusion-controlled mechanism for fluorescence blinking of colloidal quantum dots

Fluorescence blinking in nanocrystal quantum dots is known to exhibit power-law dynamics, and several different mechanisms have been proposed to explain this behavior. We have extended the measurement of quantum-dot blinking by characterizing fluctuations in the fluorescence of single dots over time scales from microseconds to seconds. The power spectral density of these fluctuations indicates a change in the power-law statistics that occurs at a time scale of several milliseconds, providing an important constraint on possible mechanisms for the blinking. In particular, the observations are consistent with the predictions of models wherein blinking is controlled by diffusion of the energies of electron or hole trap states

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