Step annealing effects on the structural and optical properties of InAs quantum dots grown on GaAs

The effects of multi-step rapid thermal annealing (RTA) for the self-assembled InAs quantum dots (QDs), which were grown by a molecular beam epitaxy (MBE), were investigated through photoluminescence (PL) and transmission electron microscopy (TEM). Postgrowth multi-step RTA was used to modify the structural and optical properties of the self-assembled InAs QDs. Postgrowth multi-step RTAs are as follows: one step (20 s at 750 °C); two step (20 s at 650 °C, 20 s at 750 °C); three step (30 s at 450 °C, 20 s at 650 °C, 20 s at 750 °C). It is found that significant narrowing of the luminescence linewidth (from 132 to 31 meV) from the InAs QDs occurs together with about 150 meV blueshift by two-step annealing, compared to as-grown InAs QDs. Observation of transmission electron microscopy (TEM) shows the existence of the dots under one- and two-step annealing but the disappearance of the dots by three-step annealing. Comparing with the samples under only one-step annealing, we demonstrate a significant enhancement of the interdiffusion in the dot layer under multi-step annealing.     

Properties of self-assembled InAs quantum dots grown by various growth techniques

The properties of self-assembled InAs quantum dots (QDs) grown by molecular beam epitaxy on GaAs substrates were investigated. The surface properties of samples were monitored by reflection high-energy electron diffraction to determine growth. Photoluminescence (PL) and transmission electron microscope (TEM) were then used to observe optical properties and the shapes of the InAs-QDs. Attempts were made to grow InAs-QDs using a variety of growth techniques, including insertion of the InGaAs strained-reducing layer (SRL) and the interruption of In flux during QD growth. The emission wavelength of InAs-QDs embedded in a pure GaAs matrix without interruption of In flux was about 1.21 μm and the aspect ratio was about 0.21. By the insertion InGaAs SRL and interruption of In flux, the emission wavelength of InAs-QDs was red shifted to 1.37 μm and the aspect ratio was 0.37. From the PL and TEM analysis, the properties of QDs were improved, particularly when interruption techniques were used.     

Self-assembled InAs quantum dots with two different matrix materials

The effects of matrix materials on the structural and optical properties of self-assembled InAs quantum dots (QDs) grown by a molecular beam epitaxy were investigated by atomic force microscopy, cross-sectional transmission electron microscopy (TEM), and photoluminescence (PL) spectroscopy. Cross-sectional TEM image indicated that the average lateral size and height of InAs QDs in a GaAs matrix on a GaAs substrate were 20.5 and 5.0 nm, respectively, which showed the PL peak position of 1.19 μm at room temperature. The average lateral size and height of InAs QDs buried in an InAlGaAs matrix on InP were 26.5 and 3.0 nm, respectively. The PL peak position for InP-based InAs QDs was around 1.55 μm at room temperature. If we only consider the size quantization effects, the difference in PL peak position between two QD systems with different matrices may be too large. The large difference in peak position can be mainly related to the QD size as well as the strain between the QDs and the matrix materials. The intermixing between the QDs and the matrix materials can partially change the In composition of QDs, resulting in the modification of the optical properties.     

Zinc oxide quantum dots embedded films by metal organic chemical vapor deposition

Zinc oxide (ZnO) quantum dots (QDs) were fabricated on silicon substrates by metal organic chemical vapor deposition. Formation of QDs is due to the vigorous reaction of the precursors when a large amount of precursors was introduced during the growth. The size of the QDs ranged from 3 to 12 nm, which was estimated by high-resolution transmission electron microscopy. The photoluminescence measured at 80 K showed that the emission of QDs embedded film ranged from 3.0 to 3.6 eV. The broad near-band-edge emission was due to the quantum confinement effect of the QDs.     

Nucleation and ripening of seeded InAs/GaAs quantum dots

We have investigated the nucleation and ripening of pairs of InAs/GaAs quantum dot layers separated by thin (2–20 nm) GaAs spacer layers. Reflection high energy electron diffraction (RHEED) measurements show that the 2D–3D transition in the second layer can occur for less than 1 monolayer deposition of InAs. Immediately after the islanding transition in the second layer chevrons were observed with included angles as low as 20° and this angle was seen to increase continuously to 45±2° as more material was deposited. Atomic force microscopy showed the dot density in both layers to be the same. It is proposed that surface morphology can radically alter processes that determine the nucleation and ripening of the 3D islands.     

Self-alignment of self-assembled InAs quantum dots

The lateral self-alignment properties of self-assembled InAs quantum dots (QDs) on a conventional GaAs (1 0 0) substrate by molecular beam epitaxy were investigated. The shape and optical properties of QDs were investigated by atomic force microscopy, transmission electron microscope, and photoluminescence (PL). Attempts were made to grow InAs-QDs using the In-interruption growth technique, in which the In flux was periodically interrupted. QDs grown without using the In-interruption growth technique were grown randomly on all regions. On the other hand, in the case of QDs grown using the In-interruption growth technique, QDs were self-aligned at the boundary between bright and dark regions, the PL intensity was increased and the PL peak position of QDs were red-shifted to 1300 nm. This represent a new technique for growing self-aligned QDs because no extra processing such as electron-beam lithography, V-grooves and surface modification by scanning tunneling microscopy is needed, and aligned QDs can be grown in situ on conventional GaAs substrates.     

Characterization of InAs quantum dots on lattice-matched InAlGaAs/InP superlattice structures

Self-assembled InAs quantum dots (QDs) in an InAlGaAs matrix, lattice-matched to InP substrate, have been grown by molecular beam epitaxy (MBE). Transmission electron microscopy (TEM), double-crystal X-ray diffraction (DCXRD) and photoluminescence (PL) are used to study their structural and optical properties. In InAs/InAlGaAs/InP system, we propose that when the thickness of InAs layer deposited is small, the random strain distribution of the matrix layer results in the formation of tadpole-shaped QDs with tails towards random directions, while the QDs begin to turn into dome-shaped and then coalesce to form islands with larger size and lower density to release the increasing misfit strain with the continuous deposition of InAs. XRD rocking curves showing the reduced strain with increasing thickness of InAs layer may also support our notion. The results of PL measurements are in well agreement with that of TEM images.     

Growth of InAs on GaAs(1 0 0) by low-pressure metalorganic chemical vapor deposition employing in situ generated arsine radicals

InAs was grown by low-pressure metalorganic chemical vapor deposition on vicinal GaAs(1 0 0) substrates misoriented by 2° toward [0 0 1]. We observed InAs crystal growth, at substrate temperatures down to 300°C, employing in situ plasma-generated arsine radicals as the arsenic source. The in situ generated arsine was produced by placing solid arsenic downstream of a microwave driven hydrogen plasma. Trimethylindium (TMIn) feedstock carried by hydrogen gas was used as the indium source. The Arrhenius plot of InAs growth rate vs. reciprocal substrate temperature displayed an activation energy of 46.1 kcal/mol in the temperature range of 300–350°C. This measured activation energy value is very close to the energy necessary to remove the first methyl radical from the TMIn molecule, which has never been reported in prior InAs growth to the best of authors’ knowledge. The film growth mechanism is discussed. The crystallinity, infrared spectrum, electrical properties and impurity levels of grown InAs are also presented.     

Evolution of ordered one-dimensional and two-dimensional InAs/InP quantum dot arrays on patterned InP (1 0 0) and (3 1 1)B substrates by self-organized anisotropic strain engineering

The formation of ordered InAs/InP quantum dot (QD) arrays is demonstrated on patterned InP (1 0 0) and (3 1 1)B substrates by the concept of self-organized anisotropic strain engineering in chemical beam epitaxy (CBE). On shallow- and deep stripe-patterned InP (1 0 0) substrates, depending on the stripe orientation, the linear one-dimensional InAs QD arrays are rotated away from their natural direction due to the presence of vicinal stepped sidewall planes modifying the self-organization process, coexisting with QD free steep side facets on the deep-patterned substrates. On shallow- and deep-patterned InP (3 1 1)B substrates only QD free side facets form with flat top and bottom areas, not affecting the natural ordering of the two-dimensional InAs QD arrays. On the deep-patterned substrates a row of dense QDs forms on top along the side facets due to their slow-growing behavior. The optical properties of the QD arrays on the patterned substrates are not degraded compared to those of arrays formed on planar substrates for both InP (1 0 0) and (3 1 1)B substrates showing the potential of self-organized anisotropic strain engineering combined with step engineering for the creation of advanced complex QD arrays and networks.     

Formation of Ge-diffusion-suppressed GaAs layers and InAs quantum dots on Ge/Si substrates

Crystal growth of GaAs layers and InAs quantum dots (QDs) on the GaAs layers was investigated on Ge/Si substrates using ultrahigh vacuum chemical vapor deposition. Ga-rich GaAs with anti-site Ga atoms grown at a low V/III ratio was found to suppress the diffusion of Ge into GaAs. S-K mode QD formation was observed on GaAs layers grown on Ge/Si substrates with Ga-rich GaAs initial layers, and improved photoluminescence from 1.3 μm-emitting InAs QDs was demonstrated.     

Difference of anisotropic structures of InAs/GaAs quantum dots between organometallic vapor-phase epitaxy and molecular beam epitaxy

The anisotropies of the baseline in and [1 1 0] of InAs quantum dots (QDs) fabricated by molecular beam epitaxy (MBE) and organometallic vapor-phase epitaxy (OMVPE) are investigated. The structural and optical difference between QDs by MBE and OMVPE are investigated through an atomic force microscopy, a transmission electron microscopy, and a photoluminescence polarization measurement. It is found that the InAs QD structural anisotropy in MBE agrees with the individual growth rate anisotropy. Moreover, it is found that the mixture of the different structural anisotropies is unique in OMVPE at low growth temperature (440°C) and the growth mode is complex. From the photoluminescence polarization measurement, the InAs QD structures which mainly contribute to the optical property are decided by the plus and minus of the polarization degree of the ground state, and it is shown that the baseline anisotropy of the QDs mainly agrees with the growth rate anisotropy.     

Shorter wavelength emission with InAs quantum dots growth directly on large bandgap quaternary (In0.68Ga0.32As0.7P0.3) barriers for high current injection efficiency

We present the growth of stacked layers of InAs quantum dots directly on high bandgap In_0.68Ga_0.32As_0.7P_0.3 (λ_g=1420 nm) barriers. The quaternary material is lattice matched to InP forming a double hetero-structure. Indium flux, number of InAs stacked layers and InGaAsP inner separation layer thickness were investigated. Photoluminescence (PL) and atomic force microscopy (AFM) analysis indicate the occurrence of gallium diffusion and the arsenic/phosphorus (As/P) exchange with the InGaAsP barriers. As a result, shorter wavelength emission is observed, making the structures suitable for telecom applications.     

Structure and optical properties of self-assembled InAs/GaAs quantum dots with In0.15Ga0.85As underlying layer

A high density of 1.02×10¹¹ cm⁻² of InAs islands with In_0.15Ga_0.85As underlying layer has been achieved on GaAs (1 0 0) substrate by solid source molecular beam epitaxy. Atomic force microscopy and PL spectra show the size evolution of InAs islands. A 1.3 μm photoluminescence (PL) from InAs islands with In_0.15Ga_0.85As underlying layer and InGaAs strain-reduced layer has been obtained. Our results provide important information for optimizing the epitaxial structures of 1.3 μm wavelength quantum dots devices.     

Sol–gel synthesis and optical properties of size controlled Indium Arsenide nanocrystals embedded in silica glasses

III–V semiconductor Indium Arsenide (InAs) nanocrystals embedded in silica glasses was synthesized by combining the sol–gel process and heat treatment in H₂ gas. The size of InAs nanocrystals can be easily controlled via changing the In and As content in the starting materials and the heating temperature in a H₂ gas atmosphere. Absorption measurements indicate a blue shift in energy with a reduction on the In and As content in the SiO₂ gel glasses as a result of quantum confinement effects. A near-infrared photoluminescence with peak at 3.40 μm was observed at 6 K under 514.5 nm Ar⁺ laser excitation from InAs nanocrystals embedded in the silica gel glasses.     

Spin-flip relaxation mechanism in self-assembled quantum dots via phonon emission

Abstract

The spin-flip relaxation time for electrons in self-assembled coupled quantum dots (SACQDs) due to emission of acoustic phonons is presented. We focus on arbitrary shaped quantum dots made with InAs embedded in a wetting layer InAs and surrounded by GaAs. The electron states are calculated using the 8-band strain dependent theory. The deformation potential and the piezo- electric acoustic phonon modes are employed to estimate the electron-phonon coupling. Spin-flip time is calculated by Fermi’s Golden Rule and its dependence on the shape of the QDs, the size and the lattice temperature is investigated.     

Formation and dissolution of InAs quantum dots on GaAs

In situ reflection high energy electron diffraction (RHEED) has been used to study the time evolution during self-assembled molecular beam epitaxy (MBE) growth of InAs quantum dots on GaAs. Using a special data acquisition technique, two characteristic time constants are determined very precisely: the time t_c up to the first appearance of InAs dots and the time t_f it takes to complete the 2D–3D transition of all islands. Surprisingly, we find that t_c increases with temperature which disagrees with a thermally activated process. In contrast to this, t_f behaves Arrhenius-like and an activation energy of E_f0.39 eV is determined. Furthermore, the sum t_c+t_f does not depend significantly on temperature and corresponds to an InAs coverage of 2.0 monolayers. A second focus of this paper is the study of dissolution of InAs dots after interruption of the As flux. From the experiments, an activation energy of 3.2 eV for desorption of In located on top of the wetting layer is determined, whereas direct desorption from the wetting layer corresponds to an activation energy of 3.4 eV.     

Stacking pattern of multi-layer InAs quantum wires embedded in In0.53Ga0.47−xAlxAs matrix layers grown lattice-matched on InP substrate

Multi-layer InAs quantum wires were grown on, and embedded in In_0.53Ga_0.47−xAl_xAs (with x=0, 0.1, 0.3 and 0.48) barrier/spacer layers lattice matched to an InP substrate. Correlated stacking of the quantum wire arrays were observed with aluminum content of 0 and 0.1. The quantum wire stacks became anti-correlated as the aluminum content was increased to 0.3 and 0.48. The origin of such stacking pattern variation was investigated by finite element calculations of the chemical potential distribution for indium on the growth front surface of the capping spacer layer. It is shown that the stacking pattern transition is determined by the combined effect of strain and surface morphology on the growth front of the spacer layers.     

CrO2 (1 0 0) and TiO2 (1 0 0) film heteroepitaxy on a BaF2 (1 1 1)/Si (1 0 0) substrate

Multi-domained heteroepitaxial rutile-phase TiO₂ (1 0 0)-oriented films were grown on Si (1 0 0) substrates by using a 30-nm-thick BaF₂ (1 1 1) buffer layer at the TiO₂–Si interface. The 50 nm TiO₂ films were grown by electron cyclotron resonance oxygen plasma-assisted electron beam evaporation of a titanium source, and the growth temperature was varied from 300 to 600 °C. At an optimal temperature of 500 °C, X-ray diffraction measurements show that rutile phase TiO₂ films are produced. Pole figure analysis indicates that the TiO₂ layer follows the symmetry of the BaF₂ surface mesh, and consists of six (1 0 0)-oriented domains separated by 30° in-plane rotations about the TiO₂ [1 0 0] axis. The in-plane alignment between the TiO₂ and BaF₂ films is oriented as [0 0 1] TiO₂ || BaF₂ or [0 0 1] TiO₂ || BaF₂ . Rocking curve and STM analyses suggest that the TiO₂ films are more finely grained than the BaF₂ film. STM imaging also reveals that the TiO₂ surface has morphological features consistent with the BaF₂ surface mesh symmetry. One of the optimally grown TiO₂ (1 0 0) films was used to template a CrO₂ (1 0 0) film which was grown via chemical vapor deposition. Point contact Andreev reflection measurements indicate that the CrO₂ film was approximately 70% spin polarized.     

Heteroepitaxy of CdTe on tilting Si(2 1 1) substrates by molecular beam epitaxy

CdTe(2 1 1)B epilayers were grown on 3 in Si(2 1 1) substrates which misoriented 0–10° toward [1 1 1] by molecular beam epitaxy (MBE). The relationship of X-ray double-crystal rocking curve (XRDCRC) FWHM and deflection angle from CdTe(2 1 1) to Si(2 1 1) was studied. For 4.2–4.5 μm CdTe, the best value of FWHM 83 arcsec was achieved while deflection angle is 2.76°. A FWHM wafer mapping indicated a good crystalline uniformity of 7.4 μm CdTe on tilting Si(2 1 1), with FWHM range of 60–72 arcsec. The shear strains of these epilayers were analyzed, using reciprocal lattice points of symmetric and asymmetric reflections measured by high-resolution multi-crystal multi-reflection X-ray diffractometer (HRMCMRXD). It was found that the shear strain angle of epilayer is effectively reduced by using proper tilting Si(2 1 1) substrate. It was also proved that the lattice parameter of CdTe(2 1 1)B is affected by the shear strain and thermal strain.     

Fabrication of 2D ordered arrays of cobalt silicide nanodots on (0 0 1)Si substrates

Two-dimensional (2D) periodic arrays of Co metal and Co silicide nanodots were successfully fabricated on (0 0 1)Si substrate by using the polystyrene (PS) nanosphere lithography (NSL) technique and thermal annealing. The epitaxial CoSi₂ was found to start growing in samples after annealing at 500 °C. The sizes of the Co silicide nanodots were observed to shrink with annealing temperature. From the analysis of the selected-area electron diffraction (SAED) patterns, the crystallographic relationship between the epitaxial CoSi₂ nanodots and (0 0 1)Si substrates was identified to be [0 0 1]CoSi₂//[0 0 1]Si and (2 0 0)CoSi₂//(4 0 0)Si. By combining the planview and cross-sectional TEM examination, the epitaxial CoSi₂ nanodots formed on (0 0 1)Si were found to be heavily faceted and the shape of the faceted epitaxial CoSi₂ nanodot was identified to be inverse pyramidal. The observed results present the exciting prospect that with appropriate controls, the PS NSL technique promises to offer an effective and economical patterning method for the growth of a variety of large-area periodic arrays of uniform metal and silicide nanostructures on different types of silicon substrates.