Integral and local density of states of InAs quantum dots in GaAs/AlGaAs heterostructure observed by ballistic electron emission spectroscopy near one-electron ground state

Density of states is studied by a ballistic electron emission microscopy/spectroscopy on self-assembled InAs quantum dots embedded in GaAs/AlGaAs heterostructure prepared by metal–organic vapor phase epitaxy. An example of integral quantum dot density of states which is proportional to superposition of a derivative of ballistic current–voltage characteristics measured at every pixel (1.05 nm×1.05 nm) of quantum dot is presented. For the two lowest observed energy levels of quantum dot (the maxima in density of states) the density of states is mapped and correlated with the shape of quantum dot. It was found that prepared quantum dots have a few peaks on their flatter top and a split of the lowest energy level can be observed. This effect can be explained by inhomogeneous (nonuniform) stress distribution in the examined quantum dot.     

Coherent longitudinal-optical ground-state phonon in CdSe quantum dots triggered by ultrafast charge migration

We observe the CdSe longitudinal-optical ground-state phonon in the electron transfer system composed of CdSe quantum dots and methylviologen directly by femtosecond absorption spectroscopy. A significant phase shift indicates that the coherent oscillations are triggered by an ultrafast charge migration, which is the consequence of an electron transfer from the photoexcited quantum dot to the molecular acceptor methylviologen. In contrast, the observed coherent phonons in isolated quantum dots stem from the frequency modulation of the quantum dot excited-state spectrum. From the probe wavelength dependence of the longitudinal-optical phonons in the electronic ground state and excited state it is possible to determine a biexciton binding energy of 35?meV.     

Coherent control of Forster energy transfer in nanoparticle molecules: energy nanogates and plasmonic heat pulses

We study how Forster energy transfer from a semiconductor quantum dot to a metallic nanoparticle can be gated using quantum coherence in quantum dots. We show this allows us to use a laser field to open the flow of the energy transfer for a given period of time (on-state) before it is switched off to about zero. Utilizing such an energy gating process it is shown that quantum-dot-metallic-nanoparticle systems (meta-molecules) can act as functional nanoheaters capable of generating heat pulses with temporal widths determined by their environmental and physical parameters. We discuss the physics behind the energy nanogates using molecular states of such meta-molecules and the resonance fluorescence of the quantum dots.     

Förster energy transfer from a semiconductor quantum well to an organic material overlayer

We predict an efficient electronic energy transfer from an excited semiconductor quantum well to optically active organic molecules of the nearby medium (substrate and/or overlayer). The energy transfer mechanism is of the F?rster type and, at semiconductor-organic distances of about 50 ?, can easily be as fast as 10-100 ps, which is about an order of magnitude shorter than the effective exciton lifetime in an isolated quantum well. In such conditions, the Wannier-Mott exciton luminescence is quenched and the organic luminescence is efficiently turned on. We consider both free as well as localized quantum well excitons discussing the dependence of the energy transfer rate on temperature and localization length. A similar mechanism for the non-radiative energy transfer to the organic overlayer molecules from unbound electron-hole pairs excited in the 2D continuum is shown to be much less competitive with respect to other relaxation channels inside the inorganic quantum well (in particular, 2D exciton formation). Received 20 July 1998     

Dynamic control of electronic states in a double quantum dot under weak dissipation conditions

The problem of the time evolution of an electron wave packet in a symmetric double quantum dot under the action of a strong alternating electric field and a slowly varying bias voltage is solved theoretically under the conditions when the electron subsystem can transfer its energy to a single resonator mode. It is shown that the possibility of energy exchange between the electron subsystem and the resonator does not hamper the formation of stable electronic states localized in the left or right quantum dot (i.e., polarized states possessing a positive or negative dipole moment). An adiabatic change in the bias voltage may alter the direction of the dipole moment of the given state (which corresponds to an electron transition from one quantum dot to the other).     

Effect of the Semiconductor Quantum Dot Shell Structure on Fluorescence Quenching by Acridine Ligand

The main line of research in cancer treatment is the development of methods for early diagnosis and targeted drug delivery to cancer cells. Fluorescent semiconductor core/shell nanocrystals of quantum dots (e.g., CdSe/ZnS) conjugated with an anticancer drug, e.g., an acridine derivative, allow real-time tracking and control of the process of the drug delivery to tumors. However, linking of acridine derivatives to a quantum dot can be accompanied by quantum dot fluorescence quenching caused by electron transfer from the quantum dot to the organic molecule. In this work, it has been shown that the structure of the shell of the quantum dot plays the decisive role in the process of photoinduced charge transfer from the quantum dot to the acridine ligand, which is responsible for fluorescence quenching. It has been shown that multicomponent ZnS/CdS/ZnS shells of CdSe cores of quantum dots, which have a relatively small thickness, make it possible to significantly suppress a decrease in the quantum yield of fluorescence of quantum dots as compared to both the classical ZnS thin shell and superthick shells of the same composition. Thus, core/multicomponent shell CdSe/ZnS/CdS/ZnS quantum dots can be used as optimal fluorescent probes for the development of systems for diagnosis and treatment of cancer with the use of anticancer compounds based on acridine derivatives.     

库仑场对量子点中强耦合束缚极化子激发态性质的影响

采用线性组合算符和幺正变换方法研究量子点中强耦合束缚极化子的振动频率、第一内部激发态能量、激发能量和共振频率的性质。讨论了这些量随量子点的有效受限长度、电子-声子耦合强度和库仑束缚势的变化关系。通过数值计算结果表明:量子点中强耦合束缚极化子的振动频率、第一内部激发态能量、激发能量和共振频率随量子点的有效受限长度的减小而迅速增大,随库仑束缚势和电子-声子的耦合强度的增加而增大。     

Photoionization cross section of a donor impurity in a two-dimensional anisotropic quantum dot

A system of an electron with a hydrogenic impurity confined in a two-dimensional anisotropic quantum dot has been investigated. We report a calculation for the binding energy of a donor impurity. The important feature of a donor impurity in a two-dimensional anisotropic quantum dot is obtained via an analysis of the binding energy. The photoionization cross section associated with intersubband transitions has been calculated. The results are presented as a function of the incident photon energy. The results show that the photoionization cross section of a donor impurity in a two-dimensional anisotropic quantum dot is strongly affected by the degree of anisotropy and the size of the quantum dot.     

磁场对非对称量子点中极化子性质的影响

采用线性组合算符和幺正变换方法研究磁场对非对称量子点中弱耦合磁极化子性质的影响.导出了非对称量子点中弱耦合磁极化子的振动频率、基态能量和基态结合能随量子点的横向和纵向有效受限长度、磁场和电子-声子耦合强度的变化关系.数值计算结果表明:非对称量子点中弱耦合磁极化子的基态能量和基态结合能随量子点的横向和纵向有效受限长度的增加而迅速增大.随回旋频率的增加而增大,随电子-声子耦合强度的增加而减小.     

Quantum size effects of CO reactivity on metallic quantum dots

We study the reactivity of a metallic quantum dot when exposed to a gas phase CO molecule. First, we perform a Newns-Anderson model calculation in which the valence electrons of the quantum dot are confined by a finite potential well and the molecule is characterized by its lowest unoccupied molecular orbital in the gas phase. A pronounced quantum size effect regarding the charge transfer between the quantum dot and molecule is observed. We then perform a first-principles calculation for a selected size interval. The quantum dot is described within the jellium model and the molecule by pseudopotentials. Our results show that the charge transfer between the quantum dot and the molecule depends critically on the size of the quantum dot, and that this dependence is intimately connected with the electronic structure. The key factor for charge transfer is the presence of states with the symmetry of the chemically active molecular orbital at the Fermi level.     

抛物量子点中弱耦合磁极化子的性质

应用线性组合算符和幺正变换方法研究了抛物量子点中磁极化子的基态性质。得出基态能和基态束缚能随有效束缚强度增大而减小,随回旋频率增大而增大。当有效柬缚强度给定,基态能量随电子-体纵光学声子耦合强度增加而减小。当有效束缚强度l0>0.3时,电子-体纵光学声子耦合强度的变化对量子点中弱耦合磁极化子的基态能量的影响变得显著。当有效束缚强度l0<0.3时,电子-体纵光学声子耦合强度的变化对基态能量影响很小。由于有效束缚强度与量子点受限强度的平方根成反比,所以量子点受限越强,基态能量、基态束缚能越大,电子一体纵光学声子耦合强度和磁场的变化对量子点的影响相对越小;当量子点受限变弱时,电子-声子耦合强度变化对量子点的影响变大,磁场对量子点的影响也变大,所以在量子点中,极化子对量子点的影响不容忽略。     

Quantum Dot Research: Current State and Future Prospects

This article reviews the current state of research involving semiconductor quantum dots, provides a brief review of the theory behind their unique properties, and an introduction explaining the importance of quantum dot research. The characteristic shifting of the band gap energy with quantum dot size, as predicted from the density of states for low-dimensional structures, allows experimental measurements to determine the extent to which quantum confinement effects play a role in the resulting properties. A few of the current techniques used to measure the presence and physical characteristics of quantum dots and their energy levels is reviewed, including transmission electron microscopy, optical transmission, and Raman and photoluminescence spectroscopy. Finally, some of the more exciting applications for quantum dots currently being researched for use in the field of optoelectronics are reviewed, including quantum dot infrared photodetectors, quantum dot lasers, and quantum dot solar cells. Comments are made on the current progress and the future prospects of quantum dot research and device applications.     

量子点双链中电子自旋极化输运性质

利用非平衡格林函数方法, 研究了与单个量子点耦合的量子点双链中电子自旋极化输运性质. 由于系统中Rashba自旋轨道耦合产生的自旋相关的相位, 电子通过上下两种路径时, 自旋不同的电子干涉情况不同, 从而导致了电极中的自旋极化流. 左右两电极间的偏压使单个量子点中的自旋积聚在很大能量区域内能够保持较大的值. 由于系统结构的左右不对称, 正负偏压下自旋积聚情况完全不同. 这些计算结果将有助于实验上设计新型的自旋电子学器件.     

声子之间相互作用对量子点中极化子性质的影响

研究了抛物量子点中弱耦合极化子的性质。采用线性组合算符和微扰法,导出了抛物量子点中极化子的基态能量。当计及电子在反冲效应中发射和吸收不同波矢的声子之间的相互作用时,讨论了对量子点中极化子的基态能量的影响。通过数值计算,结果表明,量子点中极化子基态能量随量子点的有效受限长度的减小而迅速增大,随电子-LO声子的耦合强度的增加而减少。当l₀>1.4时,声子之间的相互作用不能忽略。     

柱形量子点中弱耦合磁极化子的性质

应用线性组合算符方法和幺正变换方法,研究在抛物势作用下的柱形量子点中磁极化子的性质。对ZnS量子点的数值计算表明,量子点中磁极化子的基态能量随特征频率、回旋共振频率的增大而增加,这是由于特征频率增加时振动能量、回旋共振频率增加时外磁场中的附加能量增加所致。当特征频率(或回旋共振频率)增加到某一值时,磁极化子能量由负变为正。基态能量随柱高的减小而增加,且柱高越小,增加越快;当柱高减小到某一值时,磁极化子能量也由负变为正。总之,柱形量子点中的磁极化子,其基态能量与量子点的尺度、外磁场、特征频率等有关。