Growth of three-dimensional quantum dot crystals on patterned GaAs (0 0 1) substrates

The growth of a three-dimensional (3D) InAs quantum dot (QD) crystal on a patterned GaAs (0 0 1) substrate is demonstrated. The morphology of QDs grown on a surface patterned with shallow holes is studied as a function of the amount of deposited InAs. We observe that the QDs form in the patterned holes close to each other forming lateral QD bimolecules for InAs coverages below the commonly observed critical thickness of 1.6 monolayers. When the coverage increases, the QD bimolecules coalesce to form larger single QDs. The QDs in the holes are then capped with a Ga(Al)As spacer. The buried QD array serves as a strain template for controlling the formation site of the QDs in the second layer. By tuning the growth conditions for the second and subsequent layers, we achieve a 3D InAs QD crystal with a high degree of perfection. A detail investigation of the growth on hole patterns with different periodicities is presented.     

Electronic and optical properties of InAs/InP self-assembled quantum dots on patterned substrates

We present atomistic theory of electronic and optical properties of a single InAs quantum dot grown on a pyramidal InP nanotemplate. The shape and size of the dot is assumed to follow the nanotemplate shape and size. The electron and valence hole single particle states are calculated using atomistic effective–bond–orbital model with second nearest-neighbor interactions. The electronic calculations are coupled to separately calculated strain distribution via Bir–Pikus Hamiltonian. The optical properties of InAs dots embedded in InP pyramids are calculated by solving the many-exciton Hamiltonian for interacting electron and hole complexes using the configuration–interaction method. The effect of quantum-dot geometry on the optical spectra is investigated by a comparison between dots of different shapes.     

Growth of Ge islands on prepatterned Si (0 0 1) substrates

We report on the growth and properties of Ge islands grown on (0 0 1) Si substrates with lithographically defined two-dimensionally periodic pits. After thermal desorption and a subsequent Si buffer layer growth these pits have an inverted truncated pyramid shape. We observe that on such prepatterned substrates lens-like Ge-rich islands grow at the pit bottoms with less Ge deposition than necessary for island formation on flat substrates. This is attributed to the aggregation of Ge at the bottom of the pits, due to Ge migration from the pit sidewalls. At the later stages of growth, dome-like islands with dominant {1,1,3} or {15,3,23}, or other high-index facets [i.e. {15,3,20} facets] are formed on the patterned substrates as shown by surface orientation maps using atomic force microscopy. Furthermore, larger coherent islands can be grown on patterned substrates as compared to Ge deposition on flat ones.     

Densely packed Ge quantum dots grown on SiO2/Si substrate

We studied the growing process of Ge dots on silicon substrates covered with an ultrathin silicon dioxide buffer layer which was formed with simple chemical procedure. Uniform and densely packed (10¹¹ cm⁻²) quantum dots (QDs) were obtained by optimizing the growth parameter with the MBE method. The influence of temperature, coverage, as well as the post-annealing process, on the epitaxial and non-epitaxial nanodots formation was evaluated. Nano-sized high density quantum dots were also realized with different growing conditions, whose structural and growing mechanism were discussed under the help of SEM and RHEED results.     

Ge dots on Si (1 1 1) and (1 0 0) surfaces with SiO2 coverage: Raman study

Germanium quantum dots formed on Si (1 1 1) and (1 0 0)-oriented surfaces coated with ultra-thin oxide layers are studied using Raman spectroscopy technique. Some structural properties (height, stoichiometry and mechanical stresses) of the dots were estimated from Raman data. For analysis of the experimental data, the Raman spectra of Ge nanoclusters containing some hundreds of Ge atoms were calculated numerically. The effects of the resonance enhancement of the intensity of Raman scattering in the Ge-nanoclusters–SiO₂–Si system were discussed. The influence of the lateral sizes of Ge nano-clusters on the frequencies of phonons localized in them was studied using numerical simulation. The influence of multi-layer growth on the structure of the Ge quantum dots was investigated.     

Sensitizing effects of ZnO quantum dots on red-emitting Pr-doped SiO2 phosphor

In this study, red cathodoluminescence (CL) (λ_emission=614 nm) was observed from Pr³⁺ ions in a glassy (amorphous) SiO₂ host. This emission was enhanced considerably when ZnO quantum dots (QDs) were incorporated in the SiO₂:Pr³⁺ suggesting that the ZnO QDs transferred excitation energy to Pr³⁺ ions. That is, ZnO QDs acted to sensitize the Pr³⁺ emission. The sol–gel method was used to prepare ZnO–SiO₂:Pr³⁺ phosphors with different molar ratios of Zn to Si. The effects of the ZnO QDs concentration and the possible mechanisms of energy transfer from ZnO to Pr³⁺ are discussed. In addition, the electronic states and the chemical composition of the ZnO–SiO₂:Pr³⁺ phosphors were analyzed using X-ray photoelectron spectroscopy (XPS).     

Regular array of InGaAs quantum dots with 100-nm-periodicity formed on patterned GaAs substrates

Regular arrays of InGaAs quantum dots (QDs) with a 100-nm-periodicity have been successfully fabricated by controlling the nucleation sites on artificially prepared nano-hole arrays. The nucleation probability of a single QD at each nano-hole reached 100% by depositing InGaAs at low temperature and subsequent annealing. Four InGaAs QD layers were vertically stacked while conserving the regularity, and the stacked QD array has shown a clear photoluminescence peak at room temperature. We discuss the effects of several growth conditions on the nucleation probability of QDs.     

氧化硅缓冲层对于退火形成锗量子点的作用研究

在化学氧化得到的二氧化硅薄层覆盖的硅衬底上,室温淀积锗膜并进行后期退火处理.实验表明,不同于传统退火过程形成大岛,通过一定工艺的控制可以获得高密度(~10¹¹ cm^-2)的均匀锗量子点.研究了后期退火温度对量子点的结构影响的局部反常规律并进行了原因分析.利用拉曼和荧光光谱研究了其应力和发光特性,发现在可见(500 nm)和近红外(1350 nm)的两个光致荧光峰出现. 关键词： 锗量子点 二氧化硅 退火     

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.     

Energetics of Ge nucleation on SiO2 and implications for selective epitaxial growth

We have measured the time evolution of Ge nucleation density on SiO₂ over a temperature range of 673–973 K and deposition rates from 5.1 × 10¹³ atoms/cm² s (5 ML/min) to 6.9 × 10¹⁴ atoms/cm² s (65 ML/min) during molecular beam epitaxy. The governing equations from mean-field theory that describe surface energetics and saturation nucleation density are used to determine the size and binding energy of the critical Ge nucleus and the activation energy for Ge surface diffusion on SiO₂. The critical nucleus size is found to be a single Ge atom over substrate temperatures from 673 to 773 K, whereas a three-atom nucleus is found to be the critical size over substrate temperatures from 773 to 973 K. We have previously reported 0.44 ± 0.03 eV for the Ge desorption activation energy from SiO₂. This value, in conjunction with the saturation nucleation density as a function of substrate temperature, is used to determine that the activation energy for surface diffusion is 0.24 ± 0.05 eV, and the binding energy of the three-atom nucleus is 3.7 ± 0.1 eV. The values of the activation energy for desorption and surface diffusion are in good agreement with previous experiments of metals and semiconductors on insulating substrates. The small desorption and surface diffusion activation barriers predict that selective growth occurring on window-patterned samples is by direct impingement of Ge onto Si and ready desorption of Ge from SiO₂. This prediction is confirmed by the small integral condensation coefficient for Ge on SiO₂ and two key observations of nucleation behavior on the window-patterned samples. The first observation is the lack of nucleation exclusion zones around the windows, and second is the independence of the random Ge nucleation density on patterned versus unpatterned oxide surfaces. We also present the Ge nucleation density as a function of substrate temperature and deposition rate to demarcate selective growth conditions for Ge on Si with a window-patterned SiO₂ mask.     

Effect of GaAs(1 0 0) 2° surface misorientation on the formation and optical properties of MOCVD grown InAs quantum dots

The influence of GaAs(1 0 0) 2° substrate misorientation on the formation and optical properties of InAs quantum dots (QDs) has been studied in compare with dots on exact GaAs(1 0 0) substrates. It is shown that, while QDs on exact substrates have only one dominant size, dots on misoriented substrates are formed in lines with a clear bimodal size distribution. Room temperature photoluminescence measurements show that QDs on misoriented substrates have narrower FWHM, longer emission wavelength and much larger PL intensity relative to those of dots on exact substrates. However, our rapid thermal annealing (RTA) experiments indicate that annealing shows a stronger effect on dots with misoriented substrates by greatly accelerating the degradation of material quality.     

Photocurrent spectroscopy of indirect transitions in Ge/Si multilayer quantum dots at room temperature

Lateral photoconductivity spectra of multilayer Ge/Si heterostructures with Ge quantum dots were studied in the work proposed at room temperature. The photocurrent with minimal energy 0.48-0.56 eV that is smaller than Ge band gap was observed from such structures at the geometry of waveguide excitation. Generation of the photocurrent with the limit energy 0.48-0.56 eV was explained by spatially indirect electron transitions from heavy hole states of SiGe valence band into Δ₂-valley of the conduction band of Si surrounding. It was found out that the limit energy of such transitions decreased, as the number of SiGe quantum dot layers increased.     

Mechanisms of self-organization of Ge/Si(0 0 1) quantum dots

The effect of vertical ordering in superlattices of self-assembled Ge/Si(0 0 1) quantum dots was investigated by a combination of structural and optical characterizations via in situ reflection high-energy electron diffraction, transmission electron microscopy, atomic force microscopy and photoluminescence spectroscopy. We show that the vertical ordering observed in quantum-dot superlattices is characterized not only by the alignment of islands along the growth direction but also by a reduction of the critical thickness. The better the vertical ordering is, the more pronounced the reduction of the critical thickness will be. Such an evolution of the critical thickness could be explained by elastic strain fields induced by buried islands and propagated through the spacer layers. An important result issued from this work is the realization of superlattices in which dots can have equal size in all layers. On the other hand, experiments performed on the transformation of the island shape versus the spacer layer thickness suggest that preferential nucleation induced by surface roughness may be the main mechanism responsible for the vertical ordering observed in quantum-dot superlattices.     

The effects of thermal annealing in self-assembled Ge/Si quantum dots

The effects of thermal annealing in Si base self-assembled Ge dots have been investigated by Raman spectra and PL spectra. An obvious Raman frequency shift under different annealing temperature can be observed. There are two main effects during the annealing procession: one is the inter-diffusion of the Si and Ge quantum dots; the other is the relaxation of the elastic strain. With the calculated results, PL blue shift can be related to strain relaxation effects, and/or a general decrease of Ge content due to the Ge-Si intermixing.     

Femtosecond pulsed laser deposition of Ge quantum dot growth on Si(1 0 0)-(2 × 1)

Ge quantum dots were grown on Si(1 0 0)-(2 × 1) by femtosecond pulsed laser deposition at various substrate temperatures using a femtosecond Ti:sapphire laser. In situ reflection high-energy electron diffraction and ex situ atomic force microscopy were used to analyze the film structure and morphology. The morphology of germanium islands on silicon was studied at different coverages. The results show that femtosecond pulsed laser deposition reduces the minimum temperature for epitaxial growth of Ge quantum dots to ∼280 °C, which is 120 °C lower than previously observed in nanosecond pulsed laser deposition and more than 200 °C lower than that reported for molecular beam epitaxy and chemical vapor deposition.     

Pressure effect on optical properties of modified Gaussian quantum dots

In the present work, we intend to study the pressure effect on optical properties of spherical quantum dots by using the modified Gaussian potential. In this regard, the linear, nonlinear and total intersubband absorption coefficients and refractive index changes are investigated for different hydrostatic pressures. According to the results obtained from the present work, it is deduced that: (i) the linear, nonlinear and total refractive index changes decrease and shift towards higher energies when the pressure increases and (ii) the linear, nonlinear and total absorption coefficients increase and shift towards higher energies by increasing the pressure.     

Influence of patterning on the nucleation of Ge islands on Si and SiO2 surfaces

Surface patterning is expected to influence the nucleation site of deposited nanostructures. In the present study, clean Si and SiO₂ surfaces were patterned by a nanolithographic process using a Focused Ion Beam (FIB). Ge was evaporated in ultra high vacuum at 873 K on these substrates, resulting in the formation of island arrays. Based on scanning tunneling microscopy and atomic force microscopy images, a statistical analysis was performed in order to highlight the effect of patterning on the size distribution of islands compared to a non-patterned surface. We find that the self-organization mechanism on patterned substrates results in a very good arrangement and positioning of Ge nanostructures, depending on growth conditions and holes distance, both on Si and SiO₂ surfaces.     

Molecular-beam epitaxy on shallow mesa gratings patterned on GaAs(3 1 1)A and (1 0 0) substrates

We report on the morphology and properties of the surface formed by molecular-beam epitaxy on shallow mesa gratings on patterned GaAs(3 1 1)A and GaAs(1 0 0). On GaAs(3 1 1)A substrates, the corrugated surface formed after GaAs growth on shallow mesa gratings along is composed of monolayer high steps and (3 1 1)A terraces. These pattern induced steps which are different on opposite slopes play an important role in InAs growth on this novel template leading to distinct lateral modulation of the island distribution. On GaAs(1 0 0) substrates, growth on shallow mesa gratings along [0 1 1], [0 1 0] and is drastically sensitive to the pattern direction due to the difference of steps along [0 1 1] and .     

Ge quantum dots growth on nanopatterned Si(0 0 1) surface: Morphology and stress relaxation study

The self-organized growth of germanium quantum dots on square nanopatterned Si(0 0 1) substrates is investigated by scanning tunnelling microscopy (STM) and grazing incidence X-ray diffraction (GIXRD) techniques. A regular surface patterning in the 10-100 nm period range is obtained by etching an interface dislocation network obtained by the controlled molecular bonding of Si substrates. The depth of the silicon surface profile is increased by a double etching process. Growth experiments are performed by solid source molecular beam epitaxy (MBE), and for deep trenches, germanium growth conditions are optimized to obtain one Ge dot per Si mesa. It is shown that the trench depth and the mesa profile strongly affect the dot size and its coincidence with the initial regular surface network. Anomalous GIXRD measurements are performed to highlight the Ge elastic relaxation and intermixing during heteroepitaxial growth. We report a significant modification in the stress state of Ge dots as a function of thermal annealing after growth.     

Controlling emission wavelength from InAs self-assembled quantum dots on InP (0 0 1) during MOCVD

We studied the growth of InAs quantum dots on InP (0 0 1) substrates in a low-pressure metalorganic chemical vapor deposition by using a so-called InP ‘double-cap’ procedure. With double-capping, a photoluminescence spectrum is modified into a series of multiple peaks, where the emission peaks arise from several quantum dot families with different heights changing in a step of integer number of an InAs monolayer. Cross-sectional transmission electron micrograph observations revealed that the shape of double-capped dots is dramatically changed into a thin plate-like shape with extremely flat upper and lower interfaces, being consistent with our interpretation of the photoluminescence spectrum. We showed that the procedure was extremely useful for controlling the emission wavelength from quantum dots in an InAs/InP (0 0 1) system.