Optically active quantum dots in bottom-up nanowires

This thesis is dedicated to the discovery and progressive study of quantum emitters embedded in the shell of coaxial gallium arsenide/ aluminum gallium arsenide nanowires. The bottom-up core/shell nanowires were grown in a molecular beam epitaxy machine. During the shell growth, diffusion-driven phenomena lead to segregation effects. Gallium-rich regions are formed at the nanoscopic scale. The observation has been made that the reduced dimensionality of these regions provides true tridimensional confinement for the carriers. The recombination spectra of the electrons with the holes in what was coined shell quantum dots (shell-QDs) thus appear as sets of narrow, intense peaks. The formation of shell quantum dots is taking place on a large range of growth temperatures and nominal alloy fractions, giving freedom to engineer the growth process. The shell thickness plays an important role in the quantum dot density and total ensemble spectrum. In addition, the adjunction of an aluminum arsenide predeposition layer increasing the local curvature has been seen to foster the quantum dots formation. Single emitter spectroscopy reveals the few-particles electronic structure of quantum dots, with systematic signatures for the different degrees of occupation of the quantum dot. The shape anisotropy of the quantum dots leads to observable spin-spin interactions, which lift the degeneracy of the exciton level (one hole and one electron). Generally undesirable, this effect allows here to find that the orientation of the quantum dots in the nanowire is not hard-wired to the growth direction or to the nanowire long axis. This observation is confirmed by magneto-photoluminescence experiments. The energetic splitting and shift of the spin sublevels when an external magnetic field is applied also confirms the small size of the quantum dots. It is found that for GaAs in the strong confinement regime, the Landé coefficients of the electron and hole take opposite signs and are dependent on the angle at which the field is applied. These effects allow to tune the exciton composite Landé coefficient and could be used to reduce the splitting between the exciton spin sublevels or create optically degenerate coupled systems. Finally, the sub-nanosecond dynamics happening in the quantum dots are probed with time-correlated photon counting. It is shown that the carriers in the shell are quickly captured by the quantum dots. In addition, it is proposed that the electron population is reduced due to diffusion-assisted mechanisms or through electron-donor recombination

Exciton Footprint of Self-assembled AlGaAs Quantum Dots in Core-Shell Nanowires

Quantum-dot-in-nanowire systems constitute building blocks for advanced photonics and sensing applications. The electronic symmetry of the emitters impacts their function capabilities. Here, we study the fine structure of gallium-rich quantum dots nested in the shell of GaAs-AlGaAs core-shell nanowires. We used optical spectroscopy to resolve the splitting resulting from the exchange terms and extract the main parameters of the emitters. Our results indicate that the quantum dots can host neutral as well as charges excitonic complexes and that the excitons exhibit a slightly elongated footprint, with the main axis tilted with respect to the growth axis. GaAs-AlGaAs emitters in a nanowire are particularly promising for overcoming the limitations set by strain in other systems, with the benefit of being integrated in a versatile photonic structure

Tailoring the diameter and density of self-catalyzed GaAs nanowires on silicon

Nanowire diameter has a dramatic effect on the absorption cross-section in the optical domain. The maximum absorption is reached for ideal nanowire morphology within a solar cell device. As a consequence, understanding how to tailor the nanowire diameter and density is extremely important for high-efficient nanowire-based solar cells. In this work, we investigate mastering the diameter and density of self-catalyzed GaAs nanowires on Si(111) substrates by growth conditions using the self-assembly of Ga droplets. We introduce a new paradigm of the characteristic nucleation time controlled by group III flux and temperature that determine diameter and length distributions of GaAs nanowires. This insight into the growth mechanism is then used to grow nanowire forests with a completely tailored diameter-density distribution. We also show how the reflectivity of nanowire arrays can be minimized in this way. In general, this work opens new possibilities for the cost-effective and controlled fabrication of the ensembles of self-catalyzed III-V nanowires for different applications, in particular in next-generation photovoltaic devices

Cavity-Enhanced Photon Emission from a Single Germanium-Vacancy Center in a Diamond Membrane

The nitrogen-vacancy center in diamond has been explored extensively as a light-matter interface for quantum information applications, however it is limited by low coherent photon emission and spectral instability. Here, we present a promising interface based on an alternate defect with superior optical properties (the germanium-vacancy) coupled to a finesse $\approx11{,}000$ fiber cavity, resulting in a $31^{+11}_{-15}$-fold increase in the spectral density of emission. This work sets the stage for cryogenic experiments, where we predict a measurable increase in the spontaneous emission rate.Comment: 7 pages, 6 figure

High mechanical bandwidth fiber-coupled Fabry-Perot cavity

Fiber-based optical microcavities exhibit high quality factor and low mode volume resonances that make them attractive for coupling light to individual atoms or other microscopic systems. Moreover, their low mass should lead to excellent mechanical response up to high frequencies, opening the possibility for high bandwidth stabilization of the cavity length. Here, we demonstrate a locking bandwidth of 44 kHz achieved using a simple, compact design that exploits these properties. Owing to the simplicity of fiber feedthroughs and lack of free-space alignment, this design is inherently compatible with vacuum and cryogenic environments. We measure the transfer function of the feedback circuit (closed-loop) and the cavity mount itself (open-loop), which, combined with simulations of the mechanical response of our device, provide insight into underlying limitations of the design as well as further improvements that can be made

Mapping the directional emission of quasi-two-dimensional photonic crystals of semiconductor nanowires using Fourier microscopy

Controlling the dispersion and directionality of the emission of nanosources is one of the major goals of nanophotonics research. This control will allow the development of highly efficient nanosources even at the single-photon level. One of the ways to achieve this goal is to couple the emission to Bloch modes of periodic structures. Here, we present the first measurements of the directional emission from nanowire photonic crystals by using Fourier microscopy. With this technique, we efficiently collect and resolve the directional emission of nanowires within the numerical aperture of a microscope objective. The light emission from a heterostructure grown in each nanowire is governed by the photonic (Bloch) modes of the photonic crystal. We also demonstrate that the directionality of the emission can be easily controlled by infiltrating the photonic crystal with a high refractive index liquid. This work opens new possibilities for the control of the emission of sources in nanowires.QN/Quantum NanoscienceApplied Science

Nanoskiving Core–Shell Nanowires: A New Fabrication Method for Nano-optics

This paper describes the fabrication of functional optical devices by sectioning quantum-dotin-nanowires systems with predefined lengths and orientations. This fabrication process requires only two steps: embedding the nanowires in epoxy, and using an ultramicrotome to section them across their axis (“nanoskiving”). This work demonstrates the combination of four capabilities: i) the control of the length of the nanowire sections at the nanometer scale; ii) the ability to process the nanowires after cutting using wet etching; iii) the possibility of modifying the geometry of the wire by varying the sectioning angle; and iv) the generation of as many as 120 consecutive slabs bearing nanowires which have uniform size and approximately reproducible lateral patterns, and which can subsequently be transferred to different substrates. The quantum dots inside the nanowires are functional and of a high optical quality after the sectioning process, and exhibit photoluminescent emission with wavelengths in the range of 650-710 nm.Chemistry and Chemical Biolog