Raman scattering of InAs/AlAs quantum dot superlattices grown on (001) and (311)B GaAs surfaces

ABSTRACT: We present a comparative analysis of Raman scattering by acoustic and optical phonons in InAs/AlAs quantum dot superlattices grown on (001) and (311)B GaAs surfaces. Doublets of folded longitudinal acoustic phonons up to the fifth order were observed in the Raman spectra of (001)- and (311)B-oriented quantum dot superlattices measured in the polarized scattering geometries. The energy positions of the folded acoustic phonons are well described by the elastic continuum model. Besides the acoustic phonons, the spectra display features related to confined transverse and longitudinal optical as well as interface phonons in quantum dots and spacer layers. Their frequency positions are discussed in terms of phonon confinement, elastic stress, and atomic intermixing.     

Electronic Structure of a Hydrogenic Acceptor Impurity in Semiconductor Nano-structures

The electronic structure and binding energy of a hydrogenic acceptor impurity in 2, 1, and 0-dimensional semiconductor nano-structures (i.e. quantum well (QW), quantum well wire (QWW), and quantum dot (QD)) are studied in the framework of effective-mass envelope-function theory. The results show that (1) the energy levels monotonically decrease as the quantum confinement sizes increase; (2) the impurity energy levels decrease more slowly for QWWs and QDs as their sizes increase than for QWs; (3) the changes of the acceptor binding energies are very complex as the quantum confinement size increases; (4) the binding energies monotonically decrease as the acceptor moves away from the nano-structures’ center; (5) as the symmetry decreases, the degeneracy is lifted, and the first binding energy level in the QD splits into two branches. Our calculated results are useful for the application of semiconductor nano-structures in electronic and photoelectric devices.     

Exciton-related nonlinear optical properties in cylindrical quantum dots with asymmetric axial potential: combined effects of hydrostatic pressure, intense laser field, and applied electric field

ABSTRACT: The exciton binding energy of an asymmetrical GaAs-Ga1-xAlxAs cylindrical quantum dot is studiedwith the use of the effective mass approximation and a variational calculation procedure. Theinfluence on this quantity of the application of a direct-current electric field along the growthdirection of the cylinder, together with that of an intense laser field, is particularly considered. Theresulting states are used to calculate the exciton-related nonlinear optical absorption and opticalrectification, whose corresponding resonant peaks are reported as functions of the external probes,the quantum dot dimensions, and the aluminum molar fraction in the potential barrier regions.     

A quantum mechanical formulation of electron transport induced wind forces in metallic single-walled carbon nanotubes

In this paper the forces induced on the atoms of the lattice due an electric current (electron transport induced wind forces) are calculated based on quantum mechanics. These forces are calculated in metallic single-walled armchair carbon nanotubes (SWCNTs) from the momentum transfer between the charge carriers and the lattice in a quantum mechanical framework. Energy and phonon dispersion relations are the main input for the formulation proposed. Scattering of electrons with longitudinal acoustic and longitudinal optical phonons are considered to be the only scattering mechanisms that are responsible for the momentum exchange. The current-voltage characteristics are also predicted using the same framework and show good agreement with experimental data. The study shows that using the constant effective charge number for SWCNT is inaccurate at higher electric field forces due to saturation of the lowest energy subband. The thermal effect on the effective charge number appears to be very important, due to the increasing scattering probabilities at higher temperatures.     

The Study of Quantum Interference in Metallic Photonic Crystals Doped with Four-Level Quantum Dots

In this work, the absorption coefficient of a metallic photonic crystal doped with nanoparticles has been obtained using numerical simulation techniques. The effects of quantum interference and the concentration of doped particles on the absorption coefficient of the system have been investigated. The nanoparticles have been considered as semiconductor quantum dots which behave as a four-level quantum system and are driven by a single coherent laser field. The results show that changing the position of the photonic band gap about the resonant energy of the two lower levels directly affects the decay rate, and the system can be switched between transparent and opaque states if the probe laser field is tuned to the resonance frequency. These results provide an application for metallic nanostructures in the fabrication of new optical switches and photonic devices.     

Binding Energy of Hydrogen-Like Impurities in Quantum Well Wires of InSb/GaAs in a Magnetic Field

The binding energy of a hydrogen-like impurity in a thin size-quantized wire of the InSb/GaAs semiconductors with Kane’s dispersion law in a magnetic field B parallel to the wire axis has been calculated as a function of the radius of the wire and magnitude of B, using a variational approach. It is shown that when wire radius is less than the Bohr radius of the impurity, the nonparabolicity of dispersion law of charge carriers leads to a considerable increase of the binding energy in the magnetic field, as well as to a more rapid growth of binding energy with growth of B.     

The prediction of the effective charge number in single-walled carbon nanotubes using Monte Carlo simulation

The ensemble Monte Carlo simulation is used to calculate the electron-wind forces per unit length of single-walled carbon nanotubes under an electric field applied through the nanotube axis. The electronic system and the ionic system are decoupled from each other. The rate of momentum transferred from the electronic system to the ionic system in the form of the emission or absorption of longitudinal acoustic and longitudinal optical phonons is calculated stochastically to determine the electron-wind forces. Complete unabridged energy and phonon dispersion relations are included in order to obtain more accurate results. The effect of the temperature and the electric field magnitude on the induced forces is also taken into account. Results are compared with a prediction based on quantum mechanical integral form that calculates the electron occupation probability based on a modified Fermi–Dirac distribution. Results show a quantitative agreement between the two methods, however, the method proposed in here we believe is more accurate, because it does not make simplifications for the electron occupation probability as in the modified Fermi–Dirac distribution.     

Structure and properties of cerium phosphate and silicophosphate glasses

We report on the fabrication, properties, and structure of cerium pyrophosphate glasses and partially substituted cerium silicophosphates. In those glasses, cerium occurs predominantly as Ce(III). A combination of dynamic nuclear magnetic resonance and electrical impedance spectroscopy is used to overcome the problem of assessing cerium speciation. While optical spectroscopy is unable to quantify the ratio of Ce(III)/Ce(IV) due to spectral overlap, proxy observations of the effect of silica-for-cerium substitution on optical extinction and the shape and width of the UV band gap corroborate vibrational spectroscopic data of the structural roles of cerium and silica. While silica bonding to phosphate units appears to stabilize Ce(IV), it also impedes the polaron transport, leading to higher polaron activation energy and lower electronic conductivity. On the other hand, Ce(III) is stabilized by coordinating to P = O.     

Change of Polaron Band Width in Polystyrene Composites Containing Transition Metal Halides

Abstract

Polystyrene (PS) composite films, containing various fractions of each of NiCl₂, CoCl₂ and mixtures with Ni or Co powder, were prepared by casting method. The samples were investigated by optical and scanning electron microscopes and differential scanning calorimeter. The temperature dependence of the dc electrical resistivity was interpreted on the basis of the polaron hopping model. The hopping energy states were assumed to be arised from the previously calculated 6-fold symmetric potential barrier due to the phenyl ring rotation. The polaron band width was calculated and its dependence on the filler content was explained.     

Femtosecond studies of electron dynamics at interfaces

A delocalized electron at a metal-dielectric interface interacts with the adlayer and spatially localizes or self-traps on the femtosecond time scale into what is termed a small polaron. The dynamics can be studied by two-photon photoemission. Theoretical and experimental analyses reveal the interaction energy and the lattice vibrational mode that mediates electron localization. These results contribute to a fundamental understanding of electron behavior in weakly bonded solids and can lead to a better understanding of carrier dynamics in many different systems, including organic light-emitting diodes.     

Adsorption and binding of capping molecules for highly luminescent CdSe nanocrystals--DFT simulation studies

During CdSe nanocrystal growth, loss of surface capping molecules occurs leading to a decrease of photoluminescence (PL) quantum yield. In general, aliphatic capping molecules are applied to passivate the surface of CdSe nanocrystals to modulate the optical properties of the CdSe. In this work, two kinds of alkylamine (n-butylamine (n-BA) and n-hexylamine (n-HA)) and oleic acid (OA) were used to modify the surfaces of the CdSe nanocrystals. From the PL spectra and quantum yield analyses, we observed that the PL emission peak positions of the modified CdSe nanocrystals have blue shifted for all three capping molecules. However, the PL quantum yield of the CdSe nanocrystals increased after introduction of the alkylamine molecules, but decreased with oleic acid. The detailed mechanism was not clear until now. In this study, a density function theory (DFT) simulation was employed to demonstrate binding energy and charge analyses of CdSe with n-BA, n-HA and OA. By comparing the binding energy of the bare CdSe nanocrystals to that of the CdSe with the capping molecules, it was shown that n-BA and n-HA as capping molecules help to increase the charge on Se and decrease it on cadmium of the CdSe.     

三维石墨烯-碳纳米管复合结构热导率的分子动力学模拟

采用非平衡分子动力学方法模拟了三维石墨烯-碳纳米管复合结构的法向热导率。结果表明相比于多层石墨烯,其法向热导率提高了一个量级,其界面热阻相比碳纳米管的接触热阻降低了一个量级,但是石墨烯和碳纳米管的界面形变又阻碍了三维石墨烯-碳纳米管复合热导率的进一步提高。通过其振动态密度和重叠能进一步探究了三维石墨烯-碳纳米管复合结构结构能量的传递及声子的局域化情况。结果表明,碳管的添加激发了更多中高频声子振动参与传热,但是依然是低频声子占据主导;验证了界面处的形变是阻止法向热导率进一步提升的主要因素。     

Review of electronic and optical properties of semiconducting π‐conjugated polymers: applications in optoelectronics

A general overview of the optoelectronic properties of π‐conjugated polymers is presented. Two types of polymer are discerned: interchangeable structures of the same energy (degenerate), such as polyacetylene; and non‐degenerate polymers, such as poly(para‐phenylene). The band structures of degenerate and non‐degenerate polymers are related to their conductivities in doped and non‐doped states. In both cases, disorder and impurities play an important role in conductivity. Polarons, bipolarons and excitons are detailed with respect to doping and charge transfers. Given the fibrillic nature of these materials, the variable range hopping (VRH) law for semiconducting polymers is modified to account for metallic behaviours. Optoelectronic properties—electroluminescence and photovoltaic activity—are explained in terms of HOMO and LUMO bands, polaron‐exciton and charge movement over one or more molecules. The properties of H‐ or J‐type aggregates and their effects on transitions are related to target applications. Device structures of polymer light‐emitting diodes are explicitly linked to optimising polaron recombinations and overall quantum efficiencies. The particularly promising use of π‐conjugated polymers in photovoltaic devices is discussed. Copyright © 2004 Society of Chemical Industry     

Evaluation of Polaron Transport in Solids from First-principles

Polarons are formed in polar or ionic solids, either molecular or crystalline, due to local distortions of the lattice induced by charge carriers. Polaron hopping is the primary mechanism of charge transport in these materials, such as functional ceramic compounds, with applications in photovoltaics, thermoelectrics, two-dimensional electron gas transistors, magnetic sensors, spin valve devices, and memories. Understanding the fundamental physics of polaron hopping is, therefore, of prime technological importance. This article provides a brief physical background of polarons and their hopping mechanism, focusing on first-principles calculations of polaron properties. Herein, we review recent selected studies applying the density functional theory (DFT), and describe the merits and challenges in applying DFT for such calculations, highlighting the need to address both electronic and vibrational aspects. The vibrational component of the polaron is evaluated based on structural and total energy calculations, whereas the electronic component is derived from both total energy and electron density calculations. To address the most compelling challenge of calculating polaron properties using DFT, which is the issue of electron localization, we propose to employ calculations of selected vibrational properties, such as the sound velocity, shear modulus, and Grüneisen parameter, to represent the polaron hopping energy; all of which originate from the stiffness of inter-atomic bonds. Such methodology is expected to be more straightforward than the existing ones, however demands standardization.     

甲烷水合物声子导热及量子修正

采用平衡分子动力学方法模拟了甲烷水合物的导热,给出了30~150 K甲烷水合物的热导率。采用量子修正对分子模拟结果进行处理,可以得到更接近实验值的结果。当模拟温度低于德拜温度时,量子效应对分子模拟结果的影响较大。通过对热流自相关函数拟合得到了声学声子和光学声子的弛豫时间。结果显示,声子弛豫时间随温度增加逐渐减小,声学声子导热在水合物的导热中比重最大。随着碳氧原子之间相互作用力的增加,碳氧原子之间振动的耦合程度增加,甲烷水合物的热导率增加。     

A study of photomodulated reflectance on staircase-like,n-doped GaAs/AlxGa1?xAs quantum well structures

In this study, photomodulated reflectance (PR) technique was employed on two different quantum well infrared photodetector (QWIP) structures, which consist of n-doped GaAs quantum wells (QWs) between undoped Al_xGa_1−xAs barriers with three different x compositions. Therefore, the barrier profile is in the form of a staircase-like barrier. The main difference between the two structures is the doping profile and the doping concentration of the QWs. PR spectra were taken at room temperature using a He-Ne laser as a modulation source and a broadband tungsten halogen lamp as a probe light. The PR spectra were analyzed using Aspnes’ third derivative functional form.Since the barriers are staircase-like, the structure has different ground state energies; therefore, several optical transitions take place in the spectrum which cannot be resolved in a conventional photoluminescence technique at room temperature. To analyze the experimental results, all energy levels in the conduction and in the valance band were calculated using transfer matrix technique, taking into account the effective mass and the parabolic band approximations. A comparison of the PR results with the calculated optical transition energies showed an excellent agreement. Several optical transition energies of the QWIP structures were resolved from PR measurements. It is concluded that PR spectroscopy is a very useful experimental tool to characterize complicated structures with a high accuracy at room temperature.     

Optical excitations in stoichiometric uncapped ZnS nanostructures

We calculate the optical absorption spectra of low-energy uncapped zinc sulfide nanostructures found by global optimisation (basin-hopping/simulated annealing) using time-dependent density functional theory (TD-DFT) and compare the results with experimental spectra. We predict that for all nanostructures studied the lowest excited state found by TD-DFT corresponds to an exciton with an exciton binding energy that is much larger than that of excitons in bulk zinc sulfide. We further show that for the more symmetrical nanostructures some of the excitons are dark and that the absorption on-sets, the energy of the lowest exciton, for the different nanostructures show no clear evidence of quantum confinement. We propose that this apparent lack of quantum confinement finds its origin in the fact that the lowest exciton is not evenly spread over the whole nanostructure but shows large contributions for specific groups of atoms. Finally, we show that the predicted optical absorption spectra fit with those reported experimentally.     

Versatile Dicyanomethylene-Based Fluorescent Probes for the Detection of β-Amyloid in Alzheimer’s Disease: A Theoretical Perspective

Motivated by the growing demand for target chemosensors designed with diagnostic or therapeutic capability for fibrils related to amyloidosis diseases, we investigated in the present work the response mechanism of dicyanomethylene-based fluorescent probes for amyloid fibril using a combined approach, including molecular docking, quantum mechanics/molecular mechanics (QM/MM), and the quantum chemical method. Various binding modes for the probes in β-amyloid (Aβ) are discussed, and the fibril environment-induced molecular optical changes at the most stable site are compared to the fibril-free situation in aqueous environments. The results reveal that the fluorescence enhancement for the probes in Aβ observed experimentally is an average consequence over multiple binding sites. In particular, the conformational difference, including conjugation length and donor effect, significantly contributes to the optical property of the studied probes both in water and fibril. To further estimate the transition nature of the molecular photoabsorption and photoemission processes, the hole-electron distribution and the structural variation on the first excited state of the probes are investigated in detail. On the basis of the calculations, structure–property relationships for the studied chemosensors are established. Our computational approach with the ability to elucidate the available experimental results can be used for designing novel molecular probes with applications to Aβ imaging and the early diagnosis of Alzheimer’s disease.     

The role of dislocation-induced scattering in electronic transport in GaxIn1-xN alloys

ABSTRACT: Electronic transport in unintentionally doped GaxIn1-xN alloys with various Ga concentrations (x = 0.06, 0.32 and 0.52) is studied. Hall effect measurements are performed at temperatures between 77 and 300 K. Temperature dependence of carrier mobility is analysed by an analytical formula based on two-dimensional degenerate statistics by taking into account all major scattering mechanisms for a two-dimensional electron gas confined in a triangular quantum well between GaxIn1-xN epilayer and GaN buffer. Experimental results show that as the Ga concentration increases, mobility not only decreases drastically but also becomes less temperature dependent. Carrier density is almost temperature independent and tends to increase with increasing Ga concentration. The weak temperature dependence of the mobility may be attributed to screening of polar optical phonon scattering at high temperatures by the high free carrier concentration, which is at the order of 1014 cm-2. In our analytical model, the dislocation density is used as an adjustable parameter for the best fit to the experimental results. Our results reveal that in the samples with lower Ga compositions and carrier concentrations, alloy and interface roughness scattering are the dominant scattering mechanisms at low temperatures, while at high temperatures, optical phonon scattering is the dominant mechanism. In the samples with higher Ga compositions and carrier concentrations, however, dislocation scattering becomes more significant and suppresses the effect of longitudinal optical phonon scattering at high temperatures, leading to an almost temperature-independent behaviour.     

Donor impurity-related linear and nonlinear intraband optical absorption coefficients in quantum ring: effects of applied electric field and hydrostatic pressure

The linear and nonlinear intraband optical absorption coefficients in GaAs three-dimensional single quantum rings are investigated. Taking into account the combined effects of hydrostatic pressure and electric field, applied along the growth direction of the heterostructure, the energies of the ground and first excited states of a donor impurity have been found using the effective mass approximation and a variational method. The energies of these states are examined as functions of the dimensions of the structure, electric field, and hydrostatic pressure. We have also investigated the dependencies of the linear, nonlinear, and total optical absorption coefficients as a function of incident photon energy for several configurations of the system. It is found that the variation of distinct sizes of the structure leads to either a redshift and/or a blueshift of the resonant peaks of the intraband optical spectrum. In addition, we have found that the application of an electric field leads to a redshift, whereas the influence of hydrostatic pressure leads to a blueshift (in the case of on-ring-center donor impurity position) of the resonant peaks of the intraband optical spectrum.