Electron-phonon coupling and localization of excitons in single silicon nanocrystals

We report a detailed photoluminescence (PL) study on single silicon nanocrystals produced by laser pyrolysis. The PL spectra reveal nearly homogeneously broadened zero-phonon lines coupled to Si-O-Si phonon transitions in the SiO2 shell. A systematic investigation of electron-phonon coupling is reported on the basis of single nanocrystals. The stepwise localization of electron and hole at the Si-SiO2 interface for nanocrystals smaller than d approximately 2.7 nm is driven by electron-phonon coupling. From the localization energies the effective Bohr radii of the (localized) electron and hole are estimated to be in the range of 1-2 bond lengths of Si-O and Si-Si.     

Spectral shape dependence in the very strong coupling regime of Eliashberg theory

The effect of ² F() shape dependence on several physical properties of superconductors is studied at various values of the strong coupling indexT _c/ _ln . Our results indicate that the degree of shape dependence of each property is sensitive to the value ofT _c/ _ln . Generally, for the region we examine, 0.25T _c/ _ln 1.3, the dependence on shape is found to be higher than in the conventional strong coupling regimeT _c/ _ln 0.2. However, with the exception of the mass enhancement parameter , the amount of shape dependence does not increase steadily withT _c/ _ln and there appears to be regions of maximum shape sensitivity.     

Simultaneous spectroscopic and topographic near-field imaging of TiO2 single surface states and interfacial electronic coupling

We have probed single surface states and the involved interfacial charge transfer coupling on the TiO(2) surface using confocal as well as tip-enhanced near-field topographic-spectroscopic imaging analysis on a niobium-doped rutile TiO(2)(110) surface. The confocal images excited with a radially polarized donut mode render ring-shaped excitation patterns typical for quantum systems with two perpendicular transition dipole moments. The tip-enhanced near-field optical images of single surface states are visualized by the strong exciton plasmon-polariton coupling localized at the subdomain boundaries with a spatial resolution of ～15 nm (far beyond the optical diffraction limit). We suggest that the abundant surface states in the doped TiO(2) generate excitons under laser excitation which are strongly coupled to the surface plasmon-polaritons of the Au tip. Moreover, the interfacial electronic molecule-substrate coupling has been characterized by probing the molecule-perturbed surface states distribution and the associated specific Raman vibrational modes. The imaging and characterization of the surface states and their distributions on TiO(2) surfaces at nanoscale are critically relevant to a deep understanding of interfacial electron transfer dynamics and energetics involving in solar energy conversion, photocatalysis, and mechanistic understanding of surface-enhanced Raman scattering spectroscopy.     

Electronic density of states at the interface between silicon and lead borosilicate glass

The density-of-states distribution in the band gap of Si at the interface between Si and lead borosilicate (SiO₂-PbO-B₂O₂-Al₂O₃-Ta₂O₅) glass was assessed byC-V measurements. It is shown that reducing the temperature at which the passivating glass coating is applied decreases the interfacial density of states to a level comparable with the density of surface states on thermally oxidized Si.     

Exciton superposition states in CdSe nanocrystals measured using broadband two-dimensional electronic spectroscopy

Coherent superpositions among eigenstates are of interest in fields as diverse as photosynthesis and quantum computation. In this report, we used two-dimensional electronic spectroscopy (2D ES) to measure the decoherence time of a superposition of the two lowest-energy excitons in colloidal CdSe nanocrystals (cubic phase) in solution at room temperature. In the electron-hole representation, the quantum coherence is, remarkably, a twelve-particle correlation. By comparing the measured 2D ES to simulations, we also explored the effects of inhomogeneous broadening and examined the spectroscopic signatures of biexcitons.     

Fluctuating local field approach to the description of lattice models in the strong coupling regime

Journal of Superconductivity and Novel Magnetism - We consider 2D Hubbard clusters magnetism in the strong coupling regime. We show that the mean field approach does not provide sufficient results....     

Acceptor and surface states of ZnO nanocrystals: a unified model

Semiconductor nanocrystals have the potential for a range of applications in optoelectronics and nonlinear optics. As the surface-to-volume ratio increases, surface emission processes become more important. Using infrared (IR) and photoluminescence (PL) spectroscopy, we have developed a unified model for the acceptor and intragap surface states of ZnO nanocrystals. A PL peak was observed at 2.97?eV, in agreement with an acceptor level previously observed in the IR (Teklemichael et al 2011 Appl. Phys. Lett. 98 232112). The temperature dependence of the IR absorption peaks, which correspond to a hole binding energy of 0.46?eV, showed an ionization activation energy of only 0.08?eV. This activation energy is attributed to thermal excitation of the hole to surface states 0.38?eV above the valence band maximum. Therefore, while the acceptor is deep with respect to the bulk valence band, it is shallow with respect to surface states. A strong red PL emission centered at 1.84?eV, with an excitation onset of 3.0?eV, is attributed to surface recombination.     

Optical investigation of quantum confinement in PbSe nanocrystals at different points in the Brillouin zone

We present detailed investigations on the optical properties of PbSe nanocrystals. The absorption spectra of monodisperse, quasispherical nanocrystals exhibit sharp features as a result of distinct optical transitions. To study the size dependence, absorption spectra of nanocrystals ranging from 3.4 to 10.9 nm in diameter are analysed and a total of 11 distinct optical transitions are identified. The assignment of the various optical transitions is discussed and compared to theoretically calculated transition energies. By plotting all transitions as a function of nanocrystal size (D) we find that the energy (E) changes with the following relationship [Formula: see text] for the lowest energy transitions. The transition energy extrapolates to approximately 0.3 eV for infinite crystal size, in agreement with the bandgap of bulk PbSe at the L-point in the Brillouin zone. In addition, high-energy transitions are observed, which extrapolate to 1.6 eV for infinite crystal size, which is in good agreement with the bulk bandgap of PbSe at the Sigma-point in the Brillouin zone. Tight-binding calculations confirm that the high-energy transitions originate from the Sigma-point in the Brillouin zone. The Sigma-character of the high-energy transitions may be of importance to explain the mechanism behind multiple exciton generation in PbSe nanocrystals.     

Comparison of semiclassical and quantum models of a two-level atom-cavity QED system in the strong coupling regime

We present a numerical study comparing semiclassical and quantum models of a damped, strongly interacting cavity QED system composed of a single two-level atom interacting with a single quantized cavity mode driven externally by a tunable monochromatic field. We compute the steady state transmission spectrum of the coupled system under each model and show that in the strong coupling regime, the two models yield starkly different results. The fully quantum mechanical model of the system correctly yields the expected multiphoton transmission spectra while the semiclassical approach results in a bistable spectrum.     

Crossover between weak and strong coupling in 2D superconductors

We study the crossover between weak coupling and strong coupling in two-dimensional (2D) superconductors atT⊋0 in the weak coupling regime, described by the BCS state, and we calculate the order parameter and the chemical potential atT=0 andT⊋0 for the model of a 2D superconductor. In the strong coupling regime the energy excitation has the scale of the pairs generated by the attractive interaction. The order parameter and the chemical potential atT⊋0 are calculated, and we show that there is a continuous transition between the two regimes.     

Generation of motional entangled coherent state in an optomechanical system in the single photon strong coupling regime

The single-photon strong coupling in the deep-resolved sideband of the optomechanical system induces photon blockade (PB) effect. For the PB cavity, an initial mechanical coherent state evolves into superposition of phonon cat states entangled with the cavity Fock states. Measurement of the cavity photon number states produces phonon even and odd cat states. The information leakage effect of two photon states on the fidelity of cat states is calculated, it is shown that for low average phonon number this effect is negligible and decreases by increasing the two photon cavity state. The Lindblad equation is solved numerically to obtain the environmental effects on the fidelity of cat states.     

Imaging of localized electronic states at a nonconducting surface by single-electron tunneling force microscopy

Localized electronic states near a nonconducting SiO(2) surface are imaged on a approximately 1 nm scale by single-electron tunneling between the states and a scanning probe tip. Each tunneling electron is detected by electrostatic force. The images represent the number of tunneling electrons at each spatial location. The spatial resolution of the single electron tunneling force microscope is determined by quantum mechanical tunneling, providing new atomic-scale access to electronic states in dielectric surfaces and nonconducting nanostructures.     

An analysis of the distributions of electronic states associated with hydrogenated amorphous silicon

We study the distributions of conduction band and valence band electronic states associated with hydrogenated amorphous silicon. We find that there are substantial deviations from square-root distributions of electronic states, particularly deep within the bands and within the gap region. We clearly identify where these distributions of electronic states exhibit square-root functional dependencies by fitting square-root functional forms to some experimental data. The corresponding DOS effective masses are determined, and are found to be about 2 to 4 times greater than the crystalline silicon case.     

Resonant frequencies in the transverse vibrations of magnetic tape reels

Strength of Materials -     

Stress states and growth behavior of bridged cracks at creep regime

In this study growth behavior of bridged cracks, resulting from the growth of pre-nucleated creep cavities with diffusional and dislocation-assisted mechanisms, is investigated numerically. The elements bridging the crack are assumed to be elastic; the bridging behavior ranges from full development of the bridging zones to failure of the bridging elements during the course of crack growth. The results indicate that the bridging traction significantly relaxes even with the overall creep deformation alone. The rate of this relaxation is not influenced by the rate of crack growth. However, the rate of change in the bridging zone length or the density of the bridging elements in the bridging zone strongly affects both the maximum value and the distribution of the traction in the bridging zone. A much weaker stress singularity than the ones described by K or C^* was found ahead of the bridged cracks in the creep regime. In this weak singularity region the cavities, located at increasing distance from the crack tip, grow at similar high rates to each other.     

Second harmonic generation in the strong absorption regime

Abstract

A detailed theoretical analysis of the second harmonic generation in the strong absorption regime (great absorption index K _2w) is presented. Inside the nonlinear medium, it is found that only the harmonic wave travelling in the same direction as the fundamental one survives. Outside the nonlinear medium, the transmitted and reflected intensities of the harmonic waves show a peculiar dependence on k _2w- The ratio between transmitted and reflected intensities ranges from 5 to 75. Reflected and transmitted harmonic waves appear to be generated in the outer layers within a thickness of a fraction of wavelength. Experimental support is reported with application to a proton-exchanged LiNbO₃ waveguide.     

First-principles study of silicon nanocrystals: structural and electronic properties, absorption, emission, and doping

Total energy calculations within the Density Functional Theory have been carried out in order to investigate the structural, electronic, and optical properties of un-doped and doped silicon nanostructures of different size and different surface terminations. In particular the effects induced by the creation of an electron-hole pair on the properties of hydrogenated silicon nanoclusters as a function of dimension are discussed in detail showing the strong interplay between the structural and optical properties of the system. The distortion induced on the structure by an electronic excitation of the cluster is analyzed and considered in the evaluation of the Stokes shift between absorption and emission energies. Besides we show how many-body effects crucially modify the absorption and emission spectra of the silicon nanocrystals. Starting from the hydrogenated clusters, different Si/O bonding at the cluster surface have been considered. We found that the presence of a Si--O--Si bridge bond originates significative excitonic luminescence features in the near-visible range. Concerning the doping, we consider B and P single- and co-doped Si nanoclusters. The neutral impurities formation energies are calculated and their dependence on the impurity position within the nanocrystal is discussed. In the case of co-doping the formation energy is strongly reduced, favoring this process with respect to the single doping. Moreover the band gap and the optical threshold are clearly red-shifted with respect to that of the pure crystals showing the possibility of an impurity based engineering of the absorption and luminescence properties of Si nanocrystals.     

Correlation between stress and carrier nonradiative recombination for silicon nanocrystals in an oxide matrix

Silicon nanocrystals embedded in an oxide matrix formed in a multilayer architecture were deposited by the magnetron sputtering method. By means of Raman spectroscopy we have found that compressive stress is exerted on the silicon nanocrystal core. The stress varies as a function of silicon concentration (O/Si ratio) in the silicon-rich oxide (SRO) layers, which can be attributed to the changing nanocrystal environment. By conducting the time-resolved spectroscopy experiment, we demonstrate that, depending on the nanocrystal surroundings, a different amount of nonradiative recombination sites participates in the excited carrier relaxation process, leading to changes of the relative quantum yield of photoluminescence.     

Optical characterization of nanocrystals in silicon rich oxide superlattices and porous silicon

We propose to analyze ellipsometry data by using effective medium approximation (EMA) models. Thanks to EMA, having nanocrystalline reference dielectric functions and generalized critical point (GCP) model the physical parameters of two series of samples containing silicon nanocrystals, i.e. silicon rich oxide (SRO) superlattices and porous silicon layers (PSL), have been determined. The superlattices, consisting of ten SRO/SiO₂ layer pairs, have been prepared using plasma enhanced chemical vapor deposition. The porous silicon layers have been prepared using short monopulses of anodization current in the transition regime between porous silicon formation and electropolishing, in a mixture of hydrofluoric acid and ethanol. The optical modeling of both structures is similar. The effective dielectric function of the layer is calculated by EMA using nanocrystalline components (nc-Si and GCP) in a dielectric matrix (SRO) or voids (PSL). We discuss the two major problems occurring when modeling such structures: (1) the modeling of the vertically non-uniform layer structures (including the interface properties like nanoroughness at the layer boundaries) and (2) the parameterization of the dielectric function of nanocrystals. We used several techniques to reduce the large number of fit parameters of the GCP models. The obtained results are in good agreement with those obtained by X-ray diffraction and electron microscopy. We investigated the correlation of the broadening parameter and characteristic EMA components with the nanocrystal size and the sample preparation conditions, such as the annealing temperatures of the SRO superlattices and the anodization current density of the porous silicon samples. We found that the broadening parameter is a sensitive measure of the nanocrystallinity of the samples, even in cases, where the nanocrystals are too small to be visible for X-ray scattering. Major processes like sintering, phase separation, and intermixing have been revealed as a function of annealing of the SRO superlattices.     

Thermal conductivity of ge and ge-si core-shell nanowires in the phonon confinement regime

Heterostructure core-shell semiconductor nanowires (NWs) have attracted tremendous interest recently due to their remarkable properties and potential applications as building blocks for nanodevices. Among their unique traits, thermal properties would play a significant role in thermal management of future heterostructure NW-based nanoelectronics, nanophotonics, and energy conversion devices, yet have been explored much less than others. Similar to their electronic counterparts, phonon spectrum and thermal transport properties could be modified by confinement effects and the acoustic mismatch at the core-shell interface in small diameter NWs (<20 nm). However, fundamental thermal measurement on thin core shell NWs has been challenging due to their small size and their expected low thermal conductivity (κ). Herein, we have developed an experimental technique with drastically improved sensitivity capable of measuring thermal conductance values down to ～10 pW/K. Thermal conductivities of Ge and Ge-Si core-shell NWs with diameters less than 20 nm have been measured. Comparing the experimental data with Boltzmann transport models reveals that thermal conductivities of the sub-20 nm diameter NWs are further suppressed by the phonon confinement effect beyond the diffusive boundary scattering limit. Interestingly, core-shell NWs exhibit different temperature dependence in κ and show a lower κ from 300 to 388 K compared to Ge NWs, indicating the important effect of the core-shell interface on phonon transport, consistent with recent molecular dynamics studies. Our results could open up applications of Ge-Si core shell NWs for nanostructured thermoelectrics, as well as a new realm of tuning thermal conductivity by "phononic engineering".