Three-dimensional nanoscale study of Al segregation and quantum dot formation in GaAs/AlGaAs core-shell nanowires

GaAs/Al-GaAs core-shell nanowires fabricated by molecular beam epitaxy contain quantum confining structures susceptible of producing narrow photoluminescence (PL) and single photons. The nanoscale chemical mapping of these structures is analyzed in 3D by atom probe tomography (APT). The study allows us to confirm that Al atoms tend to segregate within the AlGaAs shells towards the vertices of the hexagons defining the nanowire cross section. We also find strong alloy fluctuations remaining AlGaAs shell, leading occasionally to the formation of quantum dots (QDs). The PL emission energies predicted in the framework of a 3D effective mass model for a QD analyzed by APT and the PL spectra measured on other nanowires from the same growth batch are consistent within the experimental uncertainties. (C) 2014 AIP Publishing LLC.

Growth and characterization of single quantum dot devices for fiber-based quantum communications

Blandine Alloing

Single photon sources have recently attracted significant interest for their potential role in the future applications of quantum cryptography, and in the longer term, quantum computing. Among the different types of single photon emitters, semiconductor quantum dots (QDs) are good candidates as they combine discrete electronic transitions with the possibility of electrical excitation. Self-assembled InAs QDs on GaAs substrate are by far the most studied system as they can easily be grown into a microcavity structure. Embedding these into a microcavity is important as it increases the extraction efficiency, directionality and speeds up the photon emission. Until now, most studies have concentrated on QDs emitting in the λ

EPFL2006

Tailored-Potential Pyramidal Quantum Dot Heterostructures

Valentina Troncale

Semiconductor quantum dots are usually compared to artificial atoms, because their electronic structure consists of discrete energy levels as for natural atoms. These artificial systems are integrated in solid materials and can be localized with a spatial precision of the order of nanometers. Besides, they conserve their quantum properties even at quite high temperatures (∼ 10 K). These properties make quantum dots one of the most suitable systems for the realization of quantum devices and computers. However, the energy states and the optical properties of quantum dots are much more complicated than for atoms, because a quantum dot is never an isolated potential well. Instead, its electronic structure depends on the crystallin structure of the semiconductor material and on the Coulomb ion-electron and electron-electron correlations. In particular, the presence of several valence bands and their mixing, induced by quantum confinement, gives rise to novel properties which are still not completely understood and exploited in applications. To get a major advance in this field, a full deterministic control of the spatial shape of the quantum confinement is needed, combined with a deeper understanding of the connections between electronic and optical properties. This thesis work has these two main objectives. We realized and experimentally studied different quantum dot systems, in pyramidal hetero-structures grown with MOCVD techniques. These systems allowed the realization of several different geometries for the carrier confining potential, with a precision in the order of nanometers. The optical characterization has been obtained in particular by means of polarization-resolved microphotoluminescence, magneto-photoluminescence, excitation photoluminescence (PLE), and interferometry techniques. For single quantum dots, we have observed and characterized for the first time new excitonic complexes, arising from excited hole states. This allowed a full caracterizatioon of the valence band hole states in our peculiar system. By means of photon correlation measurements, we have also experimentally demonstrated that, even in presence of a large family of exciton states, these quantum dot systems can emit single photons. We have then realized much more complex quantum dot structures, double dot systems (quantum dot molecules) and a completely new system called Dot-in-Dot (DiD). This latter is composed by a small inner dot surrounded by an electrostatic potential well (which can be considered as an outer elongated dot). Such a composite system is characterized by a strong valence band mixing. This state superposition is however very sensitive to small variations of the confining potential. Therefore the degree of valence band mixing can be easily switched by the introduction of a week external field. Since the valence band mixing determines the polarization properties of the emitted light, the DiD changes the polarization properties of its emission spectrum under the action of an external field. In particular, we have experimentally demonstrated this effect for an external static magnetic field, while we have numerically predicted a very similar effect for a static electric field. In the latter case, the polarization switching is a direct consequence of the quantum confined Stark effect induced in the DiD. Hence the DiD appears to be an ideal candidate for realizing emitters of single photons with tunable and controllable polarization.

EPFL2010

Scanning Tunneling Microscopy and Luminescence of Individual Nanostructures

Theresa Lutz

A detailed investigation and characterization of the local properties of individual nanoscopic structures is of great importance for the understanding of novel physical phenomena at the nanoscale as well as for the assessment of their possible use in future applications. A unique tool for the study of such structures are scanning probe methods. These methods do not only allow to obtain atomic scale information in both topographic and spectroscopic measurements at surfaces, but can also be employed for example to stimulate local photon emission. In this thesis the growth mechanism of inorganic and organic semiconductor nanostructures and the relation between their local structure and their electronic and optical properties is investigated by scanning probe techniques. In the first part of this thesis, the growth as well as the local electronic and morphologic properties of InAs/GaAs(001) quantum dots grown by molecular beam epitaxy are described. The recorded spectra show evidence of the discretization of the density of states that can be attributed to the zero dimensional confinement of charge carriers to the quantum dots. Moreover, the shape evolution of the quantum dots during the controlled removal of material through an in situ etching gas is studied. High resolution topographic images reveal that hereby an island shape transition takes place. This shape evolution is found to be the reverse of the shape evolution that typically takes place during the growth, indicating that thermodynamic factors play an important role during the growth process and the etching process. In addition, the mechanism of the material removal from the quantum dots is investigated in detail by the analysis of the size evolution of the islands as a function of the nominal amount of etched material. The second part of this thesis is dedicated to the study of individual CdSe nanowires grown by the solution-liquid-solid approach. These nanowires consist of small alternating sections of wurtzite and zincblende lattice structures. This structural arrangement also leads to an alternating electronic structure in the form of a type II band alignment along the long axis of the nanowires. The local electronic properties of the nanowires are analyzed by scanning tunneling spectroscopy. Tunneling current induced luminescence spectra from individual nanowires are acquired by the injection of holes and electrons and their subsequent radiative recombination. In contrast to previous studies on similar systems, the coupling of tip induced plasmons to the radiation process is not required. The shape and the position of the luminescence spectra is compared to photoluminescence spectra and Raman measurements. The photon energy is found to decrease with increasing wire diameter indicating quantum confinement of the charge carriers to the wire. The bulk bandgap, that can be extrapolated from the energy vs. diameter dependence of the emission peaks, indicates that the photons are emitted from zincblende type CdSe sections. Moreover, the diameter dependence reveals that the emission stems from carriers that are confined to quantum dot like parts of the wires. The lack of light emission from the wurtzite type segments is also re ected in the appearance of non-luminescent regions in the NW as shown by spatially resolved light intensity maps. Possible mechanisms for the light excitation are discussed. The investigation of single molecules of the luminescent organic emitter tris-(2-phenylpyridine)iridium(III) (Ir(ppy)3) is the topic of the last part of this thesis. To this end, Ir(ppy)3 molecules are deposited onto metal substrates and different types of thin insulating layers. Besides their structural and electronic characterization, the optical properties of single molecules are studied by tunneling current induced luminescence. No intrinsic light emission originating from the molecules can be observed neither on metal substrates nor on thin insulating layers. This indicates that in these systems, the molecules are still not sufficiently decoupled from the underlying metallic substrate. Preliminary results of tunneling current induced luminescence measurements of Ir(ppy)3 molecules on multilayers of C60 show great promise for exciting light emission on single molecules.