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 ...

On-chip single-photon sources are key components for integrated photonic quantum technologies. Semiconductor quantum dots can exhibit near-ideal single-photon emission, but this can be significantly degraded in on-chip geometries owing to nearby etched surfaces. A long-proposed solution to improve the indistinguishablility is to use the Purcell effect to reduce the radiative lifetime. However, until now only modest Purcell enhancements have been observed. Here we use pulsed resonant excitation to eliminate slow relaxation paths, revealing a highly Purcell-shortened radiative lifetime (22.7 ps) in a waveguide-coupled quantum dot-photonic crystal cavity system. This leads to near-lifetime-limited single-photon emission that retains high indistinguishablility (93.9%) on a timescale in which 20 photons may be emitted. Nearly background-free pulsed resonance fluorescence is achieved under π-pulse excitation, enabling demonstration of an on-chip, on-demand single-photon source with very high potential repetition rates.

Carrier relaxation is a key issue in determining the efficiency of semiconductor optoelectronic device operation. Devices incorporating semiconductor quantum dots have the potential to overcome many of the limitations of quantum-well-based devices because of the predicted long quantum-dot excited-state lifetimes. For example, the population inversion required for terahertz laser operation in quantum-well-based devices (quantum-cascade lasers) is fundamentally limited by efficient scattering between the laser levels, which form a continuum in the plane of the quantum well. In this context, semiconductor quantum dots are a highly attractive alternative for terahertz devices, because of their intrinsic discrete energy levels. Here, we present the first measurements, and theoretical description, of the intersublevel carrier relaxation in quantum dots for transition energies in the few terahertz range. Long intradot relaxation times (1.5 ns) are found for level separations of 14 meV (3.4 THz), decreasing very strongly to approximately 2 ps at 30 meV (7 THz), in very good agreement with our microscopic theory of the carrier relaxation process. Our studies pave the way for quantum-dot terahertz device development, providing the fundamental knowledge of carrier relaxation times required for optimum device design.

Recent developments in fabrication of van der Waals heterostructures enable new type of devices assembled by stacking atomically thin layers of two-dimensional materials. Using this approach, we fabricate light-emitting devices based on a monolayer WSe 2 , and also comprising boron nitride tunnelling barriers and graphene electrodes, and observe sharp luminescence spectra from individual defects in WSe 2 under both optical and electrical excitation. This paves the way towards the realization of electrically-pumped quantum emitters in atomically thin semiconductors. In addition we demonstrate tuning by more than 1 meV of the emission energy of the defect luminescence by applying a vertical electric field. This provides an estimate of the permanent electric dipole created by the corresponding electron-hole pair. The light-emitting devices investigated in our work can be assembled on a variety of substrates enabling a route to integration of electrically pumped single quantum emitters with existing technologies in nanophotonics and optoelectronics.The recent observation of direct bandgaps in semiconducting molybdenum and tungsten dichalcogenide monolayers has led to a rise of interest to these two-dimensional (2D) materials and demonstrated their potential for future optoelectronic devices 1,2,3,4 . These one-monolayer-thick crystals are characterised by large exciton binding energies 5,6 and oscillator strengths 7 and can be combined with other layered materials to create heterostructures held together by van der Waals forces 8,9,10,11,12 . This concept has been used to form electrically driven light-emitting structures, where MoX 2 or WX 2 (X=S or Se) monolayers were used as the exciton recombination layers, thin hexagonal boron nitride (hBN) was used for tunnelling barriers and graphene -used for transparent electrodes 11,12 .

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.