Transmission electron microscopy study of vertical quantum dots molecules grown by droplet epitaxy

The compositional distribution of InAs quantum dots grown by molecular beam epitaxy on GaAs capped InAs quantum dots has been studied in this work. Upper quantum dots are nucleated preferentially on top of the quantum dots underneath, which have been nucleated by droplet epitaxy. The growth process of these nanostructures, which are usually called as quantum dots molecules, has been explained. In order to understand this growth process, the analysis of the strain has been carried out from a 3D model of the nanostructure built from transmission electron microscopy images sensitive to the composition.     

Hole states in artificial molecules formed by vertically coupled Ge/Si quantum dots

In the tight binding approximation, the spatial configuration of the ground state and the binding energy of a hole in a “diatomic” artificial molecule formed by vertically coupled Ge/Si(001) quantum dots are studied. The inhomogeneous spatial distribution of elastic strain arising in the medium due to the lattice mismatch between Ge and Si is taken into account. The strain is calculated using the valence-force-field model with a Keating interatomic potential. The formation of the hole states is shown to be determined by the competition of two processes: the appearance of a common hole due to the overlapping of “atomic” wavefunctions and the appearance of asymmetry in the potential energy of a hole in the two quantum dots because of the superposition of the elastic strain fields from the vertically aligned Ge nanoclusters. When the thickness of the Si layer separating the Ge dots (t _Si) is greater than 2.3 nm, the binding energy of a hole in the ground state of the two-dot system proves to be lower than the ionization energy of a single quantum dot because of the partial elastic stress relaxation due to the coupling of the quantum dots and due to the decrease in the depth of the potential well for holes. For the values of the parameter t _Si, an intermediate region is revealed, where the covalent molecular bond fails and the hole is localized in one of the two quantum dots, namely, in the dot characterized by the highest strain values.     

Optical properties of InAs quantum dots in a Si matrix

We report on the optical properties of nanoscale InAs quantum dots in a Si matrix. At a growth temperature of 400°C, the deposition of 7 ML InAs leads to the formation of coherent islands with dimensions in the 2–4 nm range with a high sheet density. Samples with such InAs quantum dots show a luminescence band in the 1.3 μm region for temperatures up to 170 K. The PL shows a pronounced blue shift with increasing excitation density and decays with a time constant of 440 ns. The optical properties suggest an indirect type II transition for the InAs/Si quantum dots. The electronic structure of InAs/Si QDs is discussed in view of available band offset information.     

Spectral-luminescence properties of the complexes formed by similarly charged CdTe quantum dots and tetrasulfophthalocyanine molecules

The interaction between negatively charged CdTe quantum dots (QDs) and tetrasulfophthalocy-anine (TSPC) molecules in weak-acid and alkaline media has been investigated by spectral-luminescence methods. Similarly charged QDs and TSPC molecules are found to form complexes that exhibit energy transfer from QDs to TSPC according to the mechanism of fluorescent resonance energy transfer. The channels of QD-luminescence quenching that compete with the intracomplex energy transfer and their contribution to the total QD-luminescence quenching are discussed. A model of the formation of complexes between similarly charged QDs and molecules is proposed.     

Organic molecules passivated Mn doped Zinc Selenide quantum dots and its properties

Quantum dots of Mn doped Zinc Selenide with N-Methylaniline as the capping agent was prepared by simple and inexpensive wet chemical method. Size of the particles observed by TEM was of the order of 2-4 nm which was well consistent with the size measured by UV analysis. The presence of paramagnetic substance Mn²⁺ in the ZnSe quantum dots was confirmed by EPR measurement. Mn doped ZnSe nanoparticles exhibited a strong blue emission that was strongly dependent upon the Mn dopant level and the surface passivation produced by N-Methylaniline. The stability of the product was studied by thermal analysis which shows that this product is highly suitable for opto-electronic applications.     

Coherent dynamics in InGaAs quantum dots and quantum dot molecules

We measure the dephasing time of the exciton ground state transition in InGaAs quantum dots (QD) and quantum dot molecules (QDM) using a sensitive four-wave mixing technique. In the QDs we find experimental evidence that the dephasing time is given only by the radiative lifetime at low temperatures. We demonstrate the tunability of the radiatively limited dephasing time from 400 ps up to 2 ns in a series of annealed QDs with increasing energy separation of 69–330 meV from the wetting layer continuum. Furthermore, the distribution of the fine-structure splitting δ₁ and of the biexciton binding energy δ_B is measured. δ₁ decreases from 96 to with increasing annealing temperature, indicating an improving circular symmetry of the in-plane confinement potential. The biexciton binding energy shows only a weak dependence on the confinement energy, which we attribute to a compensation between decreasing confinement and decreasing separation of electron and hole. In the QDM we measured the exciton dephasing as function of interdot barrier thickness in the temperature range from 5 to 60 K. At 5 K dephasing times of several hundred picoseconds are found. Moreover, a systematic dependence of the dephasing dynamics on the barrier thickness is observed, showing how the quantum mechanical coupling in the molecules affects the exciton lifetime and acoustic-phonon interaction.     

Scanning tunneling microscopy observation of copper-phthalocyanine molecules on Si(100) and Si(111) surfaces

Molecules of Cu-phthalocyanine (CuPc) deposited on Si(100) and Si(111) surfaces have been observed by an ultra high vacuum field ion scanning tunneling microscope (FI-STM). On a Si(100) surface, STM images with four-fold symmetry are observed, which reflect the shape of the CuPc molecule. The STM pictures show that CuPc molecules are deposited with the molecular plane parallel to the substrate surface and have three kinds of adsorption configurations on the dimer-row of Si(100). The images of the CuPc are modified by the electronic state of the Si(100) surface. This behavior suggests strong interaction between the molecule and the substrate. The molecular images on the Si(111) surface have a unique bias-voltage dependence. At a sample bias of 1.6 V, the molecule looks transparent by STM, and becomes dark like a vacancy at 1.2 V. From the bias dependence, the electronic interaction between the CuPc molecule and the Si surface is discussed.     

Thermoelectric energy conversion in layered structures with strained Ge quantum dots grown on Si surfaces

The efficiency of the energy conversion devices depends in many ways on the materials used and various emerging cost-effective nanomaterials have promised huge potentials in highly efficient energy conversion. Here we show that thermoelectric voltage can be enhanced by a factor of 3 using layer-cake growth of Ge quantum dots through thermal oxidation of SiGe layers stacked in SiO₂/Si₃N₄ multilayer structure. The key to achieving this behavior has been to strain the Ge/Si interface by Ge dots migrating to Si substrate. Calculations taking into account the carrier trapping in the dot with a quantum transmission into the neighboring dot show satisfactory agreement with experiments above ≈200 K. The results may be of interest for improving the functionality of thermoelectric devices based on Ge/Si.     

Transport properties of quantum dots

Linear and nonlinear transport through a quantum dot that is weakly coupled to ideal quantum leads is investigated in the parameter regime where charging and geometrical quantization effects coexist. The exact eigenstates and spins of a finite number of correlated electrons confined within the dot are combined with a rate equation. The current is calculated in the regime of sequential tunneling. The analytic solution for an Anderson impurity is given. The phenomenological charging model is compared with the quantum mechanical model for interacting electrons. The current-voltage characteristics show Coulomb blockade. The excited states lead to additional fine-structure in the current voltage characteristics. Asymmetry in the coupling between the quantum dot and the leads causes asymmetry in the conductance peaks which is reversed with the bias voltage. The spin selection rules can cause a ‘spin blockade’ which decreases the current when certain excited states become involved in the transport. In two-dimensional dots, peaks in the linear conductance can be suppressed at low temperatures, when the total spins of the corresponding ground states differ by more than 1/2. In a magnetic field, an electron number parity effect due to the different spins of the many-electron ground states is predicted in addition to the vanishing of the spin blockade effect. All of the predicted features are consistent with recent experiments.     

Luminescence study of Si/Ge quantum dots

We present a photoluminescence (PL) study of Ge quantum dots embedded in Si. Two different types of recombination processes related to the Ge quantum dots are observed in temperature-dependent PL measurements. The Ge dot-related luminescence peak near 0.80 eV is ascribed to the spatially indirect recombination in the type-II band lineup, while a high-energy peak near 0.85 eV has its origin in the spatially direct recombination. A transition from the spatially indirect to the spatially direct recombination is observed as the temperature is increased. The PL dependence of the excitation power shows an upshift of the Ge quantum dot emission energy with increasing excitation power density. The blueshift is ascribed to band bending at the type-II Si/Ge interface at high carrier densities. Comparison is made with results derived from measurements on uncapped samples. For these uncapped samples, no energy shifts due to excitation power or temperatures are observed in contrast to the capped samples.     

Second-harmonic generation of semiconductor quantum dots studied by near-field optical microscopy

We present a theoretical study of optical second-harmonic generation(SHG) of symmetric semiconductor quantum dots (QDs) excited by the near field of the tip in a near-field scanning optical microscope. We show that the usual optical transition selection rules for the SH nonlinear interaction between the tip field and the QD are broken when the tip is scanned over the QD, because the tip field varies rapidly over the QD domain. It is also demonstrated that the tip-position dependence of the SH signal essentially maps the spatial distribution of the tip field.     

Micro-Raman scattering by laser-modified structures with Ge/Si quantum dots

Structures with self-assembled Ge/Si quantum dots grown by molecular-beam epitaxy are exposed to pulsed radiation of a picosecond laser. Changes in the vibrational spectrum of nanostructures under an external action are studied by Raman spectroscopy. An analysis of the Raman spectra measured with a micron spatial resolution along the exposed region indicates a mixing of Ge and Si atoms and a change in the induced mechanical stresses in quantum dots.     

Magnetic properties of quantum dots and rings

Exact many-body methods as well as current-spin-density functional theory are used to study the magnetism and electron localization in two-dimensional quantum dots and quasi-one-dimensional quantum rings. Predictions of broken-symmetry solutions within the density functional model are confirmed by exact configuration interaction (CI) calculations: In a quantum ring the electrons localize to form an antiferromagnetic chain which can be described with a simple model Hamiltonian. In a quantum dot the magnetic field localizes the electrons as predicted with the density functional approach. Received 5 December 2000     

Optical properties of InGaN quantum dots

We present time-resolved and spatially-resolved photoluminescence (PL) measurements of InGaN inclusions in a GaN matrix. The structures were grown by metal-organic chemical vapor deposition on sapphire and Si(111) substrates. Nonresonant pulsed excitation yields a broad PL peak, while resonant excitation into the nonresonant PL intensity maximum results in an evolution of a sharp resonant PL peak, having a spectral shape defined by the excitation laser pulse and a radiative decay time close to that revealed for PL under nonresonant excitation. Observation of a resonantly excited narrow PL line gives clear proof of the quantum dot (QD) nature of luminescence in InGaN–GaN samples. Cathodoluminescence (CL) and micro-PL measurements demonstrate sharp emission lines from single QD states. The recombination dynamics of single QD’s and the whole QD ensemble were investigated. Monoexponential decay was observed for the PL of single QD’s. For similar transition energies different time constants were obtained. Therefore the nonexponential decay observed for the whole ensemble is attributed to the coexistence of QD’s having similar ground-state transition energies, but significantly different electron–hole overlap.     

离子束溅射自组装Ge/Si量子点生长的演变

采用离子束溅射技术,通过改变Ge的沉积量,在n型Si(100)衬底上自组装生长了一系列Ge量子点样品. 利用AFM和Raman光谱对样品表面形貌和结构进行表征,系统地研究了Ge量子点形貌、密度、尺寸大小以及Ge的结晶性和量子点中组分等随Ge沉积量的演变规律. 结果表明:Ge层从二维薄层向三维岛过渡过程中,没有观察到传统的由金字塔形向圆顶形量子点过渡,而是直接呈圆顶形生长;且随着Ge沉积量的增加,量子点密度先增大后减小,Ge的结晶性增强同时Ge/Si互混加剧,量子点中Si的组分增加. 关键词： 离子束溅射 量子点 表面形貌 Raman光谱     

Nonlinear transport properties of quantum dots

The influence of excited levels on nonlinear transport properties of a quantum dot weakly coupled to leads is studied using a master-equation approach. A charging model for the dot is compared with a quantum mechanical model for interacting electrons. The currentvoltage curve shows Coulomb lockade and additional finestructure that is related to the excited states of the correlated electrons. Unequal coupling to the leads causes asymmetric conductance peaks. Negative differential conductances are predicted due to the existence of excited states with different spins.     

Quantum emission efficiency of nanocrystalline and amorphous Si quantum dots

The paper presents the comparison of emission efficiencies for crystalline Si quantum dots (QDs) and amorphous Si nanoclusters (QDs) embedded in hydrogenated amorphous (a-Si:H) films grown by the hot wire-CVD method (HW-CVD) at the variation of technological parameters. The correlations between the intensities of different PL bands and the volumes of Si nanocrystals (nc-Si:H) and/or an amorphous (a-Si:H) phase have been revealed using X-ray diffraction (XRD) and photoluminescence (PL) methods. These correlations permit to discuss the PL mechanisms in a-Si:H films with embedded nc-Si QDs. The QD parameters of nc-Si:H and a-Si:H QDs have been estimated from PL results and have been compared (for nc-Si QDs) with the parameters obtained by the XRD method. Using PL and XRD results the relations between quantum emission efficiencies for crystalline (η_cr) and amorphous (η_am) QDs have been estimated and discussed for all studied QD samples. It is revealed that a-Si:H films prepared by HW-CVD with the variation of wire temperatures are characterized by better passivation of nonradiative recombination centers in comparison with the films prepared at the variation of substrate temperatures or oxygen flows.     

Surface effects on the photoluminescence of Si quantum dots

Si quantum dots (SiQDs) with sizes ranging from 5 to 20 nm were fabricated by vapor condensation. They showed red photoluminescence (PL) in vacuum with the peak located at around 750 nm. After the specimen was exposed to air, the PL intensity became higher, and continued to increase during the PL test with a cycling of vacuum-air-vacuum. In pure oxygen, the PL intensity exhibited an irreversible decrease, while in nitrogen a smaller amount of reversible increase of PL intensity was observed. Furthermore, the PL intensity exhibited a remarkable enhancement if the SiQDs were treated with water. With HF treatment, the PL peak position showed a blue-shift to 680 nm, and was recovered after subsequent exposure to air. Si–O–H complexes were suggested to be responsible for this red luminescence. The irreversible decrease of PL intensity due to oxygen adsorption was speculated to be caused by the modification of chemical bonds on the surface. In the case of nitrogen adsorption, the PL change was attributed to the surface charging during adsorption.     

Electronic structure of double Ge quantum dots in Si

Theoretical investigations of the electronic structure of elastically stressed double Ge quantum dots in Si performed in the six-band kp approximation with the Bir-Pikus Hamiltonian and with the configuration interaction method are reviewed. The existence of the antibonding ground state of holes has been revealed. It has been found that, when quantum dots approach each other, the exchange energy of two-particle states has a minimum at the point of the intersection of bonding and antibonding levels; the singlet and triplet states at this point are degenerate. For the lowest spin singlet, it has been revealed that Coulomb correlations in the motion of two holes are manifested in the localization of the two-particle wavefunction at opposite quantum dots when the distance between the dots increases. It has been shown that the degree of entanglement of the singlet quantum states reaches 50% in the case of the manifestation of such spatial correlations.     

Optical absorption spectra of Si with Ge quantum dots

The results of calculations of optical absorption spectra of silicon containing Ge nanoclusters of spherical shape and different size are reported. The optical transitions from the Ge cluster levels to the silicon bulk energy band states are analyzed.