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.     

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.     

Inversion of the exciton fine structure splitting in quantum dots

The fine structure splitting of exciton state was measured for a large number of single InAs quantum dots in GaAs. It is shown to decrease as the exciton confinement decreases, crucially passing through zero and changing sign. Degeneracy of the exciton spin states is an important step to producing entangled photons from the biexciton cascade. Thermal annealing reduces the exciton confinement and thereby increases the number of degenerate dots in a particular sample.     

Time-resolved studies of single quantum dots in magnetic fields

We present time-resolved and time-integrated spectroscopy of single InAs quantum dots grown in a GaAs matrix. We observe a number of interesting features in the spectra, including the zero field splitting of exciton and biexciton lines due to quantum dot asymmetry. By the application of an in-plane magnetic field, the normally optically active and inactive exciton states become mixed, enabling us to optically probe the normally inaccessible ‘dark’ states. Time resolved measurements on the mixed states show decay times several times longer than the exciton lifetime at zero field, which we show to be consistent with a dark exciton lifetime orders of magnitude longer than that for bright exciton.     

Single-dot spectroscopy in high magnetic fields

We report on photoluminescence measurements from a single InAs/GaAs quantum dot in magnetic fields up to 28 T. Mesa-patterned structure has been used to limit the number of investigated dots. Three pairs of Zeeman-split emission lines with the same effective g*-factor and diamagnetic shift have been observed. The attribution of the lines to recombination of a neutral exciton, a biexciton, and a charged exciton is discussed.     

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.     

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     

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.     

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.     

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.     

Optical probe of InAs/GaAs self-assembled quantum dots grown using low growth rate and growth interruptions

We have investigated the optical properties of InAs/GaAs self-assembled quantum dots (QDs), grown at 500 °C using a low growth rate (0.014 ML/s), growth interruptions and a two-stage capping process. The samples exhibited large-size dots with densities in the range (3-4.5) × 10⁹ cm⁻². Macro-photoluminescence (macro-PL) measurements revealed the presence of five electronic sub-bands in the dots, with the ground state (GS) emission exhibiting a linewidth of ∼70 meV. Because of the dots large size and composition dispersions, associated with the growth method, it was possible to resolve single dots emissions using micro-PL (μ-PL) excitation in the barrier layers of the as-grown samples. The sharp PL lines were detected 60-140 meV above the GS peak energy. High-resolution resonant optical excitation of the dots PL evidenced that these fine lines originate from exciton complexes confined to the GS of individual dots. Non-resonant power dependence μ-PL spectroscopy results further confirmed the occurrence of both single exciton (X) and biexciton (XX) radiative recombinations. Finally, with increasing lattice temperature up to 95 K, PL emissions from most of these nanostructures suffered the usual thermal quenching, with activation energies (E_a) ranging between 12 and 41 meV. The relatively small values of E_a suggest that the growth technique implemented here favors the formation of defects centers in the vicinity of the QDs.     

Influence of a lateral electric field on the optical properties of InAs quantum dots

We have performed single dot photoluminescence and time-resolved ensemble photoluminescence measurements on InAs quantum dots embedded in a lateral in-plane p–i–n or n–i–n device, respectively, which makes the application of lateral electric fields, i.e. field direction perpendicular to the growth direction, feasible. Time-resolved measurements show an increase in the radiative lifetime of up to 30% with increasing field. We attribute this to the reduced overlap between the electron and hole wave functions. Single dot spectroscopy revealed a small red-shift of the emission energies of maximum 0.5 meV. This shift can be explained by the quantum confined Stark effect taking into account that the red-shift due to the band-tilting is partly compensated by a decrease in exciton binding energy.     

On Exciton Decoherence in Quantum Dots

The effects resulting due to dressing of an exciton with phonons are analyzed as the source of unavoidable decoherence of orbital degrees of freedom in quantum dots. The dressing with longitudinal optical phonons results in energetic shift of order of a few meV even of the ground state of exciton in a state-of-the-art InAs/GaAs dot and the mediating role of longitudinal acoustical phonons is essential in this process. The characteristic time needed for dressing of the exciton with optical phonons is of a picosecond order. That time can be regarded as the lower limit for decoherence for optically driven quantum gates employing self-assembled quantum dot structures.     

Photoluminescence of single quantum wires and quantum dots

The results of a study into the photoluminescence spectra of a set of quantum dots based on GaAs enclosed in AlGaAs nanowires are presented. The steady state and time resolved spectra of photoluminescence under optical excitation both from an array of quantum wires/dots and a single quantum wire/dot have been measured. In the photoluminescence spectra of single quantum dots, emission lines of excitons, biexcitons and tritons have been found. The binding energy of the biexciton in the studied structures was deduced to be 8 meV.     

Comparison of single-layer and bilayer InAs/GaAs quantum dots with a higher InAs coverage

Epitaxially grown self-assembled InAs quantum dots (QDs) have found applications in optoelectronics. Efforts are being made to obtain efficient quantum-dot lasers operating at longer telecommunication wavelengths, specifically 1.3 μm and 1.55 μm. This requires narrow emission linewidth from the quantum dots at these wavelengths. In InAs/GaAs single layer quantum dot (SQD) structure, higher InAs monolayer coverage for the QDs gives rise to larger dots emitting at longer wavelengths but results in inhomogeneous dot-size distribution. The bilayer quantum dot (BQD) can be used as an alternative to SQDs, which can emit at longer wavelengths (1.229 μm at 8 K) with significantly narrow linewidth (∼16.7 meV). Here, we compare the properties of single layer and bilayer quantum dots grown with higher InAs monolayer coverage. In the BQD structure, only the top QD layer is covered with increased (3.2 ML) InAs monolayer coverage. The emission line width of our BQD sample is found to be insensitive towards post growth treatments.     

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.     

Correlated photons from multi-carrier complexes in GaAs quantum dots

We have studied micro-photoluminescence spectra of a self-assembled single GaAs quantum dot under 8 K. With strong pulsed excitation, the micro-photoluminescence spectrum shows bright emission lines originated from an exciton, a positively charged exciton, and a biexciton, together with weak lower energy emissions reflecting multi-excitonic structures with more carriers. We have identified the origins of these weak emission lines, and showed the existence of charged biexciton states, through single photon correlation measurements and excitation power dependence of the photoluminescence intensity. In addition, investigating the radiative recombination process of the charged biexciton, we have determined the electron–hole exchange energy in the GaAs quantum dot.     

Phonon-assisted polar exciton–transitions in self-organized InAs/GaAs quantum dots

Phonon-assisted exciton transitions are investigated for self-organized InAs/GaAs quantum dots (QDs) using selectively excited photoluminescence (PL) and PL excitation spectroscopy. The results unambiguously demonstrate intrinsic recombination in the coherent InAs/GaAs QDs and the absence of a Stokes shift between ground state absorption and emission. Phonon-sidebands corresponding to a phonon energy of 34 meV are resolved and Huang–Rhys parameters of 0.015 and 0.08 are found for phonon-assisted emission and absorption, respectively, which are about one order of magnitude larger than in bulk InAs. Calculations of the exciton–LO–phonon interaction based on an adiabatic approximation and realistic wave functions for ideal pyramidal InAs/GaAs QDs show this enhanced polar coupling to result from the particular confinement and the strain-induced piezoelectric potential in such strained low-symmetry QDs.     

Bandgap engineering of self-assembled InAs quantum dots with a thin AlAs barrier

We investigate the effects of a thin AlAs layer with different position and thickness on the optical properties of InAs quantum dots (QDs) by using transmission electron microscopy and photoluminescence (PL). The energy level shift of InAs QD samples is observed by introducing the thin AlAs layer without any significant loss of the QD qualities. The emission peak from InAs QDs directly grown on the 4 monolayer (ML) AlAs layer is blueshifted from that of reference sample by 219 meV with a little increase in FWHM from 42–47 meV for ground state. In contrast, InAs QDs grown under the 4 ML AlAs layer have PL peak a little redshifted to lower energy by 17 meV. This result is related to the interdiffusion of Al atom at the InAs QDs caused by the annealing effect during growing of InAs QDs on AlAs layer.     

Resonant magnetotunneling through individual self-assembled InAs quantum dots

A single-barrier GaAs/AlAs/GaAs heterostructure, with self-assembled In-based quantum dots incorporated in the AlAs tunnel barrier, exhibits a series of resonant peaks in the low temperature current–voltage characteristics. We argue that each peak arises fromsingle-electrontunneling through thediscrete zero-dimensionalstate of anindividualInAs dot. We use the tunneling for fine probing of the local density of states in the emitter-accumulation layer. Landau-quantized states are resolved at magnetic field B∥ as low as 0.2 T. Spin-splitting of the dot electron states has been observed forB⊥I.