Control of structural and excitonic properties of self-organized InAs/GaAs quantum dots

A systematic dependence of excitonic properties on the size of self-organized InAs/GaAs quantum dots is presented. The bright exciton fine-structure splitting changes from negative values to more than 0.5 meV, and the biexciton binding energy varies from antibinding to binding, as the height of truncated pyramidal dots increases from 2 to above 9 InAs monolayers. A novel mode of metalorganic vapor phase epitaxy was developed for growing such quantum dots with precise shape control. The dots consist of pure InAs and feature heights varying in steps of complete InAs monolayers. Such dot ensembles evolve from a strained, rough two-dimensional layer with a thickness close to the critical value for the onset of the 2D–3D transition. Dots with a common height represent subensembles with small inhomogeneous broadening. Tuning of subensemble emission energy is achieved by varying the mean lateral extension of the respective QDs. Detailed knowledge of the structural properties of individual dots enable realistic k·p calculations to analyze the origin of the observed excitonic properties. The binding energies of charged and neutral excitons increase due to correlation by the gradually increasing number of bound states for increasing dot size. The monotonously increasing magnitude of the fine-structure splitting with dot size is shown to be caused by piezoelectricity. The identification of key parameters allows to tailor exciton properties, providing a major step towards the development of novel applications.     

Cancellation of fine-structure splitting in quantum dots by a magnetic field

We demonstrate control of the fine-structure splitting of the exciton emission lines in single InAs quantum dots by the application of an in-plane magnetic field. The composition of the barrier material and the size and symmetry of the quantum dot are found to determine decrease or increase in the linear polarization splitting of the dominant exciton emission lines with increasing magnetic field. This enables the selection of dots for which the splitting can to be tuned to zero, within the resolution of our experiments. General differences in the g-factors and exchange splittings are found for different types of dot.     

Onion like growth and inverted many-particle energies in quantum dots

Use of surfactants like antimony in MOCVD growth enables novel growth regimes for quantum dots (QDs). The quantum dot ensemble luminescence no longer appears as a single inhomogeneously broadened peak but shows a multi-modal structure. Quantum dot subensembles are forming which differ in height by exactly one monolayer. For the first time the systematic dependence of excitonic properties on quantum dot size and shape can be investigated in detail. Both biexcitonic binding energy and excitonic fine-structure splitting vary from large positive through zero to negative values. Correlation and piezoelectric effects explain the observations.     

Exciton polarization, fine-structure splitting, and the asymmetry of quantum dots under uniaxial stress

We derive a general relation between the fine-structure splitting (FSS) and the exciton polarization angle of self-assembled quantum dots under uniaxial stress. We show that the FSS lower bound under external stress can be predicted by the exciton polarization angle and FSS under zero stress. The critical stress can also be determined by monitoring the change in exciton polarization angle. We confirm the theory by performing atomistic pseudopotential calculations for the InAs/GaAs quantum dots. The work provides deep insight into the dot asymmetry and their optical properties and a useful guide in selecting quantum dots with the smallest FSS, which are crucial in entangled photon source applications.     

Fine structure splitting and biexciton binding energy in single self-assembled InAs/AlAs quantum dots

We report on photoluminescence investigations of individual InAs quantum dots embedded in an AlAs matrix which emit in the visible region, in contrast to the more traditional InAs/GaAs system. Biexciton binding energies, considerably larger than for InAs/GaAs dots, up to 9 meV are observed. The biexciton binding energy decreases with decreasing dot size, reflecting a possible crossover to an antibinding regime. Exciton and biexciton emission consists of linearly cross polarized doublets due to a large fine structure splitting up to 0.3 meV of the bright exciton state. With increasing exciton transition energy the fine structure splitting decreases down to zero at about 1.63 eV. Differences with InAs/GaAs QDs may be attributed to major dot shape anisotropy and/or larger confinement due to higher AlAs barriers.     

Size-dependent fine-structure splitting in self-organized InAs/GaAs quantum dots

A systematic variation of the exciton fine-structure splitting with quantum dot size in single quantum dots grown by metal-organic chemical vapor deposition is observed. The splitting increases from to as much as with quantum dot size. A change of sign is reported for small quantum dots. Model calculations within the framework of eight-band theory and the configuration interaction method were performed. Different sources for the fine-structure splitting are discussed, and piezoelectricity is pinpointed as the only effect reproducing the observed trend.     

Highly reduced fine-structure splitting in InAs/InP quantum dots offering an efficient on-demand entangled 1.55-microm photon emitter

To generate entangled photon pairs via quantum dots (QDs), the exciton fine-structure splitting (FSS) must be comparable to the exciton homogeneous linewidth. Yet in the (In,Ga)As/GaAs QD, the intrinsic FSS is about a few tens microeV. To achieve photon entanglement, it is necessary to cherry-pick a sample with extremely small FSS from a large number of samples or to apply a strong in-plane magnetic field. Using theoretical modeling of the fundamental causes of FSS in QDs, we predict that the intrinsic FSS of InAs/InP QDs is an order of magnitude smaller than that of InAs/GaAs dots, and, better yet, their excitonic gap matches the 1.55 microm fiber optic wavelength and, therefore, offers efficient on-demand entangled photon emitters for long distance quantum communication.     

Hydrostatic pressure effects on exciton states in InAs/GaAs quantum dots

Based on the effective-mass approximation, the hydrostatic pressure effects on exciton states in InAs/GaAs self-assembled quantum dots (QDs) are studied by means of a variational method. Numerical results show that the exciton binding energy has a minimum with increasing dot height for any hydrostatic pressure. The interband emission energy increases when the hydrostatic pressure increases. In particular, we find that hydrostatic pressure has a remarkable effect on exciton states for small QD size. Our results are in agreement with experiment measurements.     

Fine structure of the exciton states in InAs quantum dots

The fine structure of the exciton states in InAs quantum dots grown by the Stranski-Krastanov method with short growth interruptions has been studied by microphotoluminescence at cryogenic temperatures. It has been demonstrated that, with increasing quantum-dot size, the splitting of the exciton states increases steadily to ～10² μeV. It has been shown that, in the exciton energy range of 1.3–1.4 eV, the magnitude of this splitting is comparable to the natural width of the exciton lines. This result is important for the development of entangled photon pair emitters based on InAs quantum dots.     

Optical study of single InAs on In0.12Ga0.88As self-assembled quantum dots: biexciton binding energy dependence on the dots size

Single self-assembled InAs quantum dots embedded in a In_0.12Ga_0.88As quantum well and emitting in the near infrared have been optically investigated. The dependence on the excitation power of the single quantum dot photoluminescence has been used to identify the emission of the biexciton complex. The biexciton binding energy, which has been measured for a dozen dots, increases with increasing exciton transition energy for the dot sizes investigated in the present work, as a consequence of stronger confinement in a smaller quantum dot. The obtained data is compared with experimental results available in the literature for InAs quantum dots. PACS 78.67.Hc; 73.21.La; 78.55.Cr     

Quantum-dot size dependence of exciton fine-structure splitting

A systematic variation of the exciton fine-structure splitting with quantum dot size in single MOCVD-grown self-organized InAs/GaAs quantum dots is observed, ranging from several tens to as much as , thus covering more than one order of magnitude. Piezoelectricity is identified to be the dominant factor governing the observed trend. A change in sign of the fine-structure splitting is reported for the first time, originating from quantum dots with confinement potentials elongated in the and crystal direction, respectively.     

Prediction of an excitonic ground state in InAs/InSb quantum dots

Using atomistic pseudopotential and configuration-interaction many-body calculations, we predict an excitonic ground state in the InAs/InSb quantum-dot system. For large dots, the conduction band minimum of the InAs dot lies below the valence band maximum of the InSb matrix. Due to quantum confinement, at a critical size calculated here for various shapes, the gap E(g) between InAs conduction states and InSb valence states vanishes. Strong electron-hole correlation effects are induced by the spatial proximity of the electron and hole wave functions, and by the lack of strong (exciton unbinding) screening, afforded by the existence of discrete 0D confined energy levels. These correlation effects overcome E(g), leading to the formation of a biexcitonic ground state (two electrons in InAs and two holes in InSb) being energetically more favorable (by approximately 15 meV) than the dot without excitons.     

Raman coherence beats from entangled polarization eigenstates in InAs quantum dots

The homodyne-detected transient four-wave-mixing response of InAs/GaAs self-assembled quantum dots shows temporal oscillations of the optically induced Raman coherence arising from two entangled polarization eigenstates of the exciton. The phase sensitive nature of the homodyne detection enables us to follow the time evolution of the nonradiative quantum coherence between the polarization states, providing a measurement of the fine-structure splitting in the dots, which is much less than the inhomogeneous broadening, and the corresponding decoherence rate of the entangled state.     

Surface integral determination of built-in electric fields and analysis of exciton binding energies in nitride-based quantum dots

We present a simple analytical approach to calculate the built-in strain-induced and spontaneous piezoelectric fields in nitride-based quantum dots (QDs) and then apply the method to describe the variation of exciton, biexciton and charged exciton energy with dot size in GaN/AlN QDs. We first present the piezoelectric potential in terms of a surface integral over the QD surface, and confirm that, due to the strong built-in electric field, the electrons are localised near the QD top and the holes are localised in the wetting layer just below the dot. The strong localisation and smaller dielectric constant results in much larger Coulomb interactions in GaN/AlN QDs than in typical InAs/GaAs QDs, with the interaction between two electrons, J_ee, or two holes, J_hh, being about a factor of three larger. The electron–hole recombination energy is always blue shifted in the charged excitons, X⁻ and X⁺, and the biexciton, and the blue shift increases with increasing dot height. We conclude that spectroscopic studies of the excitonic complexes should provide a useful probe of the structural and piezoelectric properties of GaN-based QDs.     

Growth conditions effects on optical properties of InAs quantum dots grown by molecular beam epitaxy on GaAs (1 1 3)A substrate

We have investigated the optical properties of InAs/GaAs (1 1 3)A quantum dots grown by molecular beam epitaxy (MBE) with different growth rates by photoluminescence spectroscopy (PL) as a function of the excitation density and the sample temperature (10–300 K). Reflection high-energy electron diffraction (RHEED) is used to investigate the formation process of InAs quantum dots (QDs). A redshift of the InAs QDs PL band emission was observed when the growth rate was increased. This result was explained by the increase of the InAs quantum dot size with increasing growth rate. A significant redshift was observed when the arsenic flux was decreased. The evolution of the PL peak energy with increasing temperature has showed an S-shaped form due to the localization effects and is attributed to the efficient relaxation process of carriers in different InAs quantum dots and to the exciton transfer localized at the wetting layer.     

Millisecond fluorescence in InAs quantum dots embedded in AlAs

The temperature dependence of steady-state and time-resolved photoluminescence from self-assembled InAs quantum dots embedded in AlAs has been studied. Millisecond-long nonexponential photoluminescence decay is observed in the temperature range of 4.2–50 K. At higher temperatures, the decay time decreases to a few nanoseconds. The experimental results are interpreted using a model of singlet–triplet splitting of exciton levels in small dots in a dense quantum dot system with local carrier transfer between dots.     

Self-organized formation of shell-like InAs/GaAs quantum dot ensembles

Formation of a multimodal quantum dot (QD) ensemble by strained layer epitaxy of InAs on GaAs near the critical value for the onset of the 2D-3D transition is studied. Reflection anisotropy spectroscopy is employed to confirm that a smooth surface is maintained during strained layer growth prior to QD formation. Instantaneous capping after deposition leads to InAs quantum wells with some thickness flucuations. Multimodal QD InAs ensembles form after an at least short growth interruption prior to cap layer deposition. The QDs consist of pure InAs with heights varying in steps of complete InAs monolayers. Related exciton energies indicate a simultaneous increase of both height and lateral extension, i.e. a shell-like increase of sizes. The formation of the multimodal QD ensemble is described by a kinetic approach. A growth scenario is presented where QDs having initially shorter base length stop vertical growth at a smaller height, accounting for the experimentally observed shell-like sub-ensemble structure.     

Influence of Mg Composition on Optical Properties of Exciton Confinement in Strained Wurtzite ZnO/MgxZn1-xO Cylindrical Quantum Dots

Based on the effective-mass approximation and variational approach, excitonic optical properties are investigated theoretically in strained wurtzite (WZ) ZnO/Mg_xZn_1-xO cylindrical quantum dots (QDs) for four different Mg compositions: x=0.08, 0.14, 0.25, and 0.33, with considering a three-dimensional carrier confinement in QDs and a strong built-in electric field effect due to the piezoelectricity and spontaneous polarization. The ground-state exciton binding energy, the interband emission wavelength, and the radiative lifetime as functions of the QD structural parameters (height and radius) are calculated in detail. The computations are performed in the case of finite band offset. Numerical results elucidate that Mg composition has a significant influence on the exciton states and optical properties of ZnO/Mg_xZn_1-xO QDs. The ground-state exciton binding energy increases with increasing Mg composition and the increment tendency is more prominent for small height QDs. As Mg composition increases, the interband emission wavelength has a blue-shift if the dot height L<3.5 nm, but the interband emission wavelength has a red-shift when L>3.5 nm. Furthermore, the radiative lifetime increases rapidly with increasing Mg composition if the dot height L>3 nm and the increment tendency is more prominent for large height QDs. The physical reason has been analyzed in depth.     

Influence of Mg Composition on Optical Properties of Exciton Confinement in Strained Wurtzite ZnO/Mg_x Zn_(1-x) O Cylindrical Quantum Dots

Based on the effective-mass approximation and variational approach, excitonic optical properties are investigated theoretically in strained wurtzite (WZ) ZnO/Mg x Zn 1-x O cylindrical quantum dots (QDs) for four different Mg compositions: x = 0.08, 0.14, 0.25, and 0.33, with considering a three-dimensional carrier confinement in QDs and a strong built-in electric field effect due to the piezoelectricity and spontaneous polarization. The ground-state exciton binding energy, the interband emission wavelength, and the radiative lifetime as functions of the QD structural parameters (height and radius) are calculated in detail. The computations are performed in the case of finite band offset. Numerical results elucidate that Mg composition has a significant influence on the exciton states and optical properties of ZnO/Mg x Zn 1 x O QDs. The ground-state exciton binding energy increases with increasing Mg composition and the increment tendency is more prominent for small height QDs. As Mg composition increases, the interband emission wavelength has a blue-shift if the dot height L 3.5 nm, but the interband emission wavelength has a red-shift when L 3.5 nm. Furthermore, the radiative lifetime increases rapidly with increasing Mg composition if the dot height L 3 nm and the increment tendency is more prominent for large height QDs. The physical reason has been analyzed in depth.     

Experimental demonstration of coherent coupling of two quantum dots

During the recent years semiconductor nanostructures have attracted considerable interest with respect to potential applications in quantum information processing. In particular, quantum dot molecules have been suggested to provide the building block of a quantum computer: forming quantum gates due to coherent coupling of two dots. The characteristic dependence of the splitting of ‘bonding’ and ‘anti-bonding’ states suggests coherent coupling of two InAs/GaAs quantum dots. Anti-crossings in the fine structure of excitons due to mixing of optically bright and dark states have been observed in Faraday configuration. In Voigt configuration the diamagnetic shift of the quantum dot molecule is enhanced compared to a single quantum dot. These findings altogether demonstrate the coherent coupling of exciton states in quantum dot molecules.