No description available.

The objective of this thesis is to explore the synthesis and characterization of high quality binary ZnTe nanowires with great potential for development of optoelectronic devices including high efficiency photovoltaic cells for energy conversion and high sensitivity photodetectors for green fluorescent protein bioimaging at single molecule level. To systematically explore the fabrication process for high quality nanowires, a chemical vapour deposition system was built for nanowire growth. Computational fluid dynamics simulations were used to optimize the reactor and growth parameters. The simulations were validated by experimental measurements. Room temperature photoluminescence measurements showed that high crystal quality with very low defects by single step growth was achieved. This single step growth technique makes a great improvement compared to the reported growth followed by annealing, which achieved equivalent crystal quality. This simplification could be of use in large scale synthesis of nanowires. The simulation results also showed that reactant species concentration is a key factor influencing the growth. A metal-organic chemical vapour deposition system was thus built to independently control reactant concentrations for ZnTe nanowire growth. Temperature-dependent photoluminescence measurements of as-grown ZnTe nanowires showed a strong near band-edge emission. In addition, a deep level oxygen-related band was observed for the first time. From the detailed analysis of thermal quenching of the photoluminescence, it was shown that the deep level emission was partially from the intermediate band of the material. This is of great importance due to the theoretical absorption efficiency that is as high as 63% for intermediate band materials, which is more than two times of that of current single junction concentrators, and few materials possessing this property. Individual ZnTe nanowires, grown after optimization, were patterned and contacted, and their conductivity and photoconductivity were measured at room temperature. A single ZnTe nanowire serving as a photodetector was shown to have the highest reported visible responsivity of 360 A/W (at 530 nm), and a gain of 8,640 (at 3 V bias). The responsivity is roughly 18 times higher than that of silicon avalanche photodiodes. This demonstrates that ZnTe nanowires are strong candidates for single photon detection.

The objective of this thesis is to explore the synthesis and characterization of high quality binary ZnTe nanowires with great potential for development of optoelectronic devices including high efficiency photovoltaic cells for energy conversion and high sensitivity photodetectors for green fluorescent protein bioimaging at single molecule level. To systematically explore the fabrication process for high quality nanowires, a chemical vapour deposition system was built for nanowire growth. Computational fluid dynamics simulations were used to optimize the reactor and growth parameters. The simulations were validated by experimental measurements. Room temperature photoluminescence measurements showed that high crystal quality with very low defects by single step growth was achieved. This single step growth technique makes a great improvement compared to the reported growth followed by annealing, which achieved equivalent crystal quality. This simplification could be of use in large scale synthesis of nanowires. The simulation results also showed that reactant species concentration is a key factor influencing the growth. A metal-organic chemical vapour deposition system was thus built to independently control reactant concentrations for ZnTe nanowire growth. Temperature-dependent photoluminescence measurements of as-grown ZnTe nanowires showed a strong near band-edge emission. In addition, a deep level oxygen-related band was observed for the first time. From the detailed analysis of thermal quenching of the photoluminescence, it was shown that the deep level emission was partially from the intermediate band of the material. This is of great importance due to the theoretical absorption efficiency that is as high as 63% for intermediate band materials, which is more than two times of that of current single junction concentrators, and few materials possessing this property. Individual ZnTe nanowires, grown after optimization, were patterned and contacted, and their conductivity and photoconductivity were measured at room temperature. A single ZnTe nanowire serving as a photodetector was shown to have the highest reported visible responsivity of 360 A/W (at 530 nm), and a gain of 8,640 (at 3 V bias). The responsivity is roughly 18 times higher than that of silicon avalanche photodiodes. This demonstrates that ZnTe nanowires are strong candidates for single photon detection.

A systematic investigation into the growth of one-dimensional nanostructures of select II-VI compounds with the wurtzite crystal structure. Two process parameters are systematically altered to observe how each affects deposition. The results of which give a further understanding into the formation of one nanostructure over another, as well as experimental parameters for optimizing the growth of particular CdSe nanomaterials. A statistical analysis is conducted on the experimental data to quantitatively determine the variability and robustness of the experimental setup and process. The information complied from this extensive study will yield a more complete understanding of the experimental setup and how improvements can be made to reduce variability, increase yield, and gain insight into the mechanisms controlling this class of materials.

The hot carrier dynamics of Zn0.91Cd0.09Se/ZnSe multi-quantum wells were studied using the femtosecond time-resolved photoluminescence upconversion technique. The carrier cooling behavior was investigated for different compositions at various lattice temperatures. The hot carriers generated photoexcitation by 405nm Ti:sapphire laser pulses release their excess energy primarily through carrier-LO-phonon interaction. As the excess energy reduce to the amount that lower than the energy of LO phonon, the excess energy was released by carrier-TA-phonon scattering before radiative recombination occurs. We have determined the scattering times of carrier-LO-phonon scattering at different lattice temperatures. No hot phonon effects was found at low photoexcited carrier density. The dependence of photoluminescence lifetime on wavelength was also discussed.

No description available.

We report the possibility to control the tilting of nanoneedles and nanowires by using structured sapphire substrates. The advantage of the reported strategy is to obtain well oriented growth along a single direction tilted with respect to the surface normal, whereas the growth in other directions is suppressed. In our particular case, the nanostructures are tilted with respect to the surface normal by an angle of 58°. Moreover, we demonstrate that variation of the nanostructures shape from nanoneedles to cylindrical nanowires by using SiO2 layer is observed.

Les nanostructures de semiconducteurs II-VI ont de nombreuses applications en microélectronique, optoélectronique et photonique. Notamment, les boites quantiques II-V peuvent servir de source de photons uniques. Dans cette étude, nous nous sommes intéressés à la caractérisation chimique et structurale des nanostructures de semiconducteurs II-VI (boites quantiques (BQs) auto-organisées, nanofils II-VI et III-V …) par sonde atomique tomographique (SAT). Dans un premier temps, nous avons optimisé les conditions d’analyse des semiconducteurs III-V et II-VI par SAT. Ensuite, nous avons étudié les compositions chimiques des interfaces II-VI/III-V en montrant la formation d’un composé Ga2.7Se3 à l’interface ZnSe/GaAs et un mélange de cations (Ga, Zn) à l’interface ZnTe/InAs. Les mesures de compositions chimiques et des tailles des boites quantiques en trois dimensions par SAT ont permis de faire une corrélation avec les mesures optiques. Nous nous sommes aussi intéressés à l’étude des mécanismes de croissance des nanofils GaAs et ZnTe ainsi que des BQs (CdTe) insérés dans des nanofils ZnTe en analysant la composition chimique des catalyseurs, les BQs dans les nanofils aussi que la base des nanofils. Ces mesures montrent que les boites quantiques sont formées d’un fort mélange CdxZn1-xTe. Un scénario basé sur la diffusion de surface a été proposé pour expliquer la croissance ainsi que le mélange entre Zn/Cd pour les BQs insérées dans les nanofils. / Nanostructures of II-VI nanostructure have many applications in microelectronics, optoelectronics and photonics. For example, II -V quantum dots have shown the ability to be a source of single photons. In this work, we performed in the chemical and structural characterization of nanostructures of II-VI semiconductors (self- organized quantum dots (QDs), nanowires II-VI and III- V ...) by atom probe tomography (APT). Firstly, the analysis conditions of III-V and II- VI semiconductors by APT were optimized. Then, we studied the chemical composition of II-VI/III-V interfaces and showed the formation of a Ga2.7Se3 compound at the ZnSe/GaAs interface and the (Ga, Zn) cations mixing at the ZnTe/InAs interface. The measurements of the chemical composition and the sizes of quantum dots in three dimensions by APT allowed making a correlation with optical measurements. We studied also growth mechanisms of GaAs, ZnTe nanowire and the CdTe QDs inserted in ZnTe nanowires by analyzing the chemical composition of the catalysts QDs and nanowires basis. These measurements show that the quantum dots are formed of a strong mixing of CdxZn1-xTe. A scenario based on surface diffusion has been proposed to explain the growth and the mixing between Zn/Cd for the QDs.

Halbleiter Quantenpunkte (QP) standen in den letzten Jahren im Mittelpunkt vieler Forschungsaktivitäten im Bezug auf mögliche Anwendungen im Bereich der Quanteninformationsverarbeitung. Durch das dreidimensional Confinement sind nur diskrete, energetisch stark separierte Zustände in einem QP möglich. Damit sind phasenzerstörende Streuprozesse unwahrscheinlicher und man kann Dekohärenzzeiten erwarten, die nur durch die Lebensdauer der Zustände limitiert sind. Materialbasis dieser Arbeit sind CdSe QP in einer ZnSe Barriere. In dieser Arbeit werden zwei Arten von Kohärenzphenomänen, die das zeitliche Verhalten solcher Quantensysteme beschreiben, mittels optischer Methoden untersucht. Im Falle optischer Kohärenz wechselwirkt ein angeregter Zustand, der strahlend mit einem Grundzustand verbunden ist, mit einem externen elektro-magnetischen Feld. Mittels phasensynchronisierter kohärenter Kontrolle werden biexzitonische und auch erste angeregte Zustände in einzelnen QP untersucht. Im Fall des angeregten Zustandes findet man optische Dephasierungszeiten unterhalb von 10 ps. Für das Biexziton kann nur eine untere Grenze bestimmt werden, die auf einer 10 ps Zeitskala liegt. Das zweite Phenomän ist die Quantenkohärenz (QK), die das Phasengedächtnis zweier Zustände im selben QP vergleicht. In dieser Arbeit wird die QK durch die Analyse von Quantenschwebungen in der Emission des Grundzustandsexzitons in einem einzelnen QP untersucht. Es wurde gefunden, dass es keine messbare Dekohärenz der beiden Unterzustände des Grundzustandsexzitons im Rahmen der strahlenden Lebensdauer von circa 300 ps gibt. Die dritte Gruppe von Experimenten beschäftigt sich mit der longitudinalen Spinrelaxationszeit einzelner Ladungsträger. Die verwendeten Proben ermöglichen den direkten Zugang zur Spindynamik einzelner Löcher. Die Experimente in der Spektral- als auch in der Zeitdomäne lieferten Spinrelaxationszeiten für Löcher von knapp 10 ns. / Semiconductor quantum dots (QD) have attracted considerable interest during the past years as possible candidates for quantum information processing. Due to the confinement potential in such structures, the density of states in a single QD is discrete. If the states are well separated in energy the coupling to the environment is expected to be smaller, implying that coherence is maintained during the exciton lifetime. In the present work CdSe in ZnSe QDs are used. Two kinds of coherence phenomena, reflecting the time evolution of such a quantum system, are studied by use of optical methods. In case of optical coherence, an excited state which is radiatively coupled to a ground state interacts with an external electro-magnetic field. The experimental technique of temporal coherent control is applied via a two photon process on the biexciton state and also by a single photon process on the excited state in a single QD. As a result optical coherence times below 10 ps are found for the excited state, while for the biexciton only a lower limit on a 10 ps timescale was elaborated. The second phenomena is quantum coherence and describes the phase memory between two states in the same QD. It is studied in this work by the analysis of the observed quantum beats in the time resolved photoluminescence emission (PL) of the ground state exciton in a single QD. As a result it was found that there is no measurable decoherence between the two substates of the ground state exciton during the exciton lifetime of about 300 ps. In a third group of experiments the longitudinal spin relaxation time is investigated on a single carrier level. The used QD sample contains charged QDs with resident electrons, which provide direct access to the separate spin dynamic of the holes. Different experiments carried out, yielding a longitudinal spin relaxation time for a single hole on a 10 ns timescale.

Halbleiter-Quantenpunkte sind Objekte in der Größenordnung von Nanometern, in denen wenige Ladungsträger in alle drei Raumrichtungen durch eine Potentialbarriere eingesperrt sind. Dies führt zu einer reduzierten Wechselwirkung mit dem Halbleiter-Gitter und zu einer diskreten Zustandsdichte. Die große Polarität der Bindung dazu, dass viele Wechselwirkungen direkt durch Spektroskopie der Photolumineszenz zu beobachten sind, was sie für die Grundlagenforschung attraktiv macht. Die ungleiche Anzahl von Elektronen und Löchern erlaubt die Untersuchung einzelner, ungepaarter Ladungsträger. Mit Hilfe der polarisationsaufgelösten Mikro-PL Spektroskopie werden Spinzustände einzelner QP reproduzierbar untersucht. Im Mittelpunkt stehen dabei Wechselwirkungen der Teilchen untereinander. Über die Anregungsspektroskopie werden höherangeregte Zustände identifiziert und charakterisiert. Die hier auftretenden Austauschwechselwirkungen führen zur Mischung zu Feinstrukturen im Spektrum. Kopplungen im angeregten Lochzustand zeigen die Möglichkeit zur optischen Orientierung des residenten Elektrons auf. Die Spinkonfiguration der Elektronen im Triplettzustand erlaubt es, die Elektron-Loch Austauschwechselwirkungen des Trions zu untersuchen. Der zweite Teil dieser Arbeit befasst sich mit semimagnetischen QP. Hier sorgt die Wechselwirkung mit einer paramagnetischen Umgebung von Manganspins für neue magneto-optische Eigenschaften. Diese zeigen sich auf der Ebene einzelner QP in Form von Linienverbreiterungen durch Spinfluktuationen als auch durch den Riesen-Zeeman-Effekt am QP-Ensemble. Besonderes Augenmerk liegt hier auf dem Einfluss der reduzierten Dimensionalität und der größeren Oberflächen der QP auf die Austauschmechanismen. Die starke Temperaturabhängigkeit der Spinumgebung wird ausgenutzt, um das Spinaufheizen als auch die Spin-Gitter-Relaxationsystematisch zu studieren. Dabei wird die PL der QP als Monitor benutzt. / Semiconductor quantum dots are objects on the nanometer scale, where charge carriers are confined in all three dimensions. This leads to a reduced interaction with the semiconductor lattice and to a discrete density of states. In the examined QD in II-VI seminconductor systems the large polar character of the bindings enables to observe particle interactions by spectroscopy of the photo-luminescence, making QD attractive for basic research. An odd number of carriers allows to study the latter in an unpaired state. By using polarization-resolved micro-PL spectroscopy, the spin-states of single, isolated QD can be studied reproducibly. Of special interest are exchange interactions in this few-particle system named trion. By excitation spectroscopy energetically higher states can be identified and characterized. The exchange interactions appearing here lead to state mixing and fine structure patterns in the spectra. Couplings in excited hole states show the way to the optical orientation of the resident electron spin. The spin configuration of the trion triplet state can be used to optically control the resident electron spin. Semimagnetic QD are focused in the second part of this work. The interaction with a paramagnetic environment of manganese spins leads to new magneto-optical properties of the QD. They reveal on a single dot level by line broadening due to spin fluctuations and by the giant Zeeman effect of the dot ensemble. Of special interest in this context is the influence of the reduced system dimension and the relatively larger surface of the system on the exchange mechanisms. The strong temperature dependence of the spin environment is used to systematically study the spin-lattice relaxation. Here, the PL of the QD ensemble monitors the spin temperature. The time constants in the mu range define the range for the incoherent switching of the Mn magnetization.