New information on the electron-hole wave functions in InAs-GaAs self-assembled quantum dots is deduced from Stark effect spectroscopy. Most unexpectedly it is shown that the hole is localized towards the top of the dot, above the electron, an alignment that is inverted relative to the predictions of all recent calculations. We are able to obtain new information on the structure and composition of buried quantum dots from modeling of the data. We also demonstrate that the excited state transitions arise from lateral quantization and that tuning through the inhomogeneous distribution of dot energies can be achieved by variation of electric field. 68.90. + g, 73.50.Pz, Self-assembled InAs-GaAs quantum dots (QDs) provide nearly ideal examples of zero-dimensional semiconductor systems [1] and are hence of considerable contemporary interest for the study of new physics and potential device applications. However, very little is known experimentally about the nature of the QD carrier wave functions and their response to applied fields. Numerous calculations of the electronic structure of QDs have been performed [2][3][4][5], but in the absence of definitive structural information they assume idealized QD shapes, usually pyramidal [6]. However there is evidence that in many cases the dots more closely approximate to lens shaped [7], and may also contain significant concentrations of Ga [8], rather than being pure InAs. In view of the uncertainties in shape and composition, the applicability of the calculated electronic structure to real dots must at best be regarded as approximate at the present time.Consequently, experimental information on the nature of the wave functions is urgently required, to provide a reliable guide to theory, and a firm basis for the interpretation of experiments. In this paper we demonstrate that photocurrent spectroscopy under electric field F provides important, new information on the carrier wave functions, and by comparison with theory, on the composition, shape and effective height of the dots. We show that the QDs possess a permanent dipole moment, implying a finite spatial separation of the electron and hole for F 0. Contrary to the predictions of all recent calculations, we demonstrate that the holes are localized above the electrons in the QDs. This "inverted" alignment can only be explained by assuming nonuniform Ga incorporation in the nominally InAs QDs. As a result of our work the extensive previous theoretical modeling of the electronic structure of InAs QDs will need to be reexamined.Two types of dots were studied, both grown by molecular-beam epitaxy on ͑001͒ GaAs substrates at 500 ± C. The first type (samples A C) was deposited at 0.01 monolayers per second (ML͞s) to give a density ഠ1.5 3 10 9 cm 22 , base size 18 nm, and height 8.5 nm [ Fig. 1(a)], as determined from transmission electron microscopy (TEM). The second type (sample D) had a higher deposition rate of 0.4 ML͞s, resulting in a density ഠ5 3 10 10 cm 22 and size 15 3 3.5 nm. The asymmetric shaped QDs, sitting on an ...
We show that by illuminating an InGaAs/GaAs self-assembled quantum dot with circularly polarized light, the nuclei of atoms constituting the dot can be driven into a bistable regime, in which either a threshold-like enhancement or reduction of the local nuclear field by up to 3 Tesla can be generated by varying the intensity of light. The excitation power threshold for such a nuclear spin "switch" is found to depend on both external magnetic and electric fields. The switch is shown to arise from the strong feedback of the nuclear spin polarization on the dynamics of spin transfer from electrons to the nuclei of the dot.The hyperfine interaction in solids [1] arises from the coupling between the magnetic dipole moments of nuclear and electron spins. It produces two dynamical effects: (i) inelastic relaxation of electron spin via the "flip-flop" process ( Fig.1a) and (ii) the Overhauser shift of the electron energy [2]. Recently, the hyperfine interaction in semiconductor quantum dots (QDs) has attracted close attention [3,4,5,6,7,8,9,10,11,12,13,14] fuelled by proposals for QD implementation in quantum information applications [15]. The full quantization of the electron states in QDs is beneficial for removing decoherence mechanisms present in extended systems [16,17]. However, the electron localization results in a stronger (than in a bulk material) overlap of its wave-function with a large number of nuclei (N ∼ 10 4 in small selfassembled InGaAs/GaAs dots and up to 10 5 ÷ 10 6 in electrostatically-defined GaAs QDs), and the resulting hyperfine interaction with nuclear spins has been found to dominate the decoherence [3,4,5,12,13,14] and life-time [9] of the electron spin at low temperatures.In this Letter, we report the observation of a pronounced bistable behaviour of nuclear spin polarisation, S, in optically pumped self-assembled InGaAs/GaAs dots. In our experiments, spin-polarized electrons are introduced one-by-one into an individual InGaAs dot at a rate w x (see Fig.1b) by the circularly polarized optical excitation of electron-hole pairs 120 meV above the lowest QD energy states. Due to hole spin-flip during its energy relaxation, both bright and dark excitons can form in the dot ground state. The former will quickly recombine radiatively with a rate w rec ≈ 10 9 sec −1 , whereas the dark exciton can recombine with simultaneous spin transfer to a nucleus via a spin "flip-flop" process (as in Fig.1a) at the rate w rec N p hf [12,18]. Here N is the number of nuclei interacting with the electron and p hf is the probability of a "flip-flop" process, which from our perturbation theory treatment is given by:(1) Here γ is the exciton life-time broadening, h hf is the strength of the hyperfine interaction of the electron with a single nucleus and E eZ is the electron Zeeman splitting. E eZ is strongly dependent on the effective nuclear magnetic field B N generated by the nuclei. This provides a feedback mechanism between the spin transfer rate and the degree of nuclear polarization (B N ∝ S) in the dot [19]. Th...
The effects of excess electron occupation on the optical properties of excitons ͑X͒ and biexcitons (2X) in a single self-assembled InGaAs quantum dot are investigated. The behavior of X and 2X differ strongly as the number of excess electrons is varied with the biexciton being much more weakly perturbed as a result of its filled s-shell ground state, a direct manifestation of shell-filling effects. Good correlation is found between charging thresholds observed from s-shell recombination perturbed by p-shell occupation, and direct observation of p-shell recombination.
Photoluminescence and complementary photocurrent spectroscopy, both as a function of electric field, are used to probe carrier capture and escape mechanisms in InAs/GaAs quantum dots. Carrier capture from the GaAs matrix is found to be highly field sensitive, being fully quenched in fields of only 15 kV/cm. For fields less than 20 kV/cm, carriers excited in the wetting layer are shown to be captured by the dots very effectively, whereas for fields in excess of 50 kV/cm tunnel escape from the wetting layer into the GaAs continuum is dominant. For excitation directly into the dots, radiative recombination dominates up to 100 kV/cm.
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