Ce travail de thèse porte sur l'étude optique de nanofils de GaN et de microcavités d'AlN contenant des boîtes quantiques de GaN. La largeur de raie de l'exciton lié au donneur neutre dans le spectre de photoluminescence des nanofils de GaN crûs par épitaxie par jets moléculaires met en evidence l'homogénéité des contraintes dans le matériau. S'ils ne présentent aucun confinement excitonique, la géométrie filaire permet une relaxation efficace des contraintes et permet d'étudier précisément le bord de bande du GaN relaxé en phase cubique. Par ailleurs, nous infirmons l'attribution de la transition à 3.45 eV observée dans le spectre des nanofils de GaN wurtzite à un satellite à deux électrons. En effet, les règles de sélection de son dipôle, ainsi que son évolution sous champ magnétique intense, montrent que cette transition n'a pas les propriétés d'un satellite à deux électrons. Nous avons également étudié la spectroscopie de microdisques d'AlN contenant des boîtes quantiques de GaN. Des facteurs de qualité record pour les cavités en AlN ont été mesurés autour de 3 eV. Des nanocavités d'AlN contenues dans des guides d'onde unidimensionnels ont également été étudiées. L'attribution de chaque mode au guide d'onde ou à la cavité, prédite par des calculs préliminaires, est confirmée expérimentalement par une localisation différente. Ces structures donnent lieu à d'excellents facteurs de qualité, de 2300 à 3.45 eV, jusqu'à 4400 à 3.14 eV. Si le facteur de Purcell attendu est très élevé (autour de 100), nous n'avons pas réussi à observer l'effet Purcell. Ceci s'explique soit par l'instabilité des modes de cavité et de l'émission des boîtes quantiques sous exposition prolongée, soit par l'importance des recombinaisons non radiatives. Enfin, il apparaît que le frein principal à l'obtention de l'effet laser dans ces structures est l'important champ électrique interne, qui ralentit l'émission spontanée des boîtes quantiques.

Ce travail de thèse s'inscrit dans le contexte de la fonctionnalisation de matériaux cellulosiques dans le domaine de l'électronique imprimée. Une première approche a mis en évidence la possibilité d'imprimer des formulations aqueuses à base de nanoparticules de polymères semi-conducteurs photoluminescents. L'influence de la taille des nanoparticules, ainsi que leur composition (ajout d'un polymère dérive de la cellulose) sur la couleur de l'émission a été mise en évidence. Les applications potentielles peuvent être l'élaboration de papiers sécurisés. Une seconde approche s'est portée sur l'utilisation de microfibrilles de cellulose et de microparticules de cuivre afin d'élaborer des films composites conducteurs autoportants grâce aux excellentes propriétés mécaniques des microfibrilles. L'influence d'un calandrage (pression et température de calandrage) des films sur la conductivité électrique a en particulier été étudiée.

Die vorliegende Arbeit befasst sich mit dem vertieften Verständnis der Rekombinationsdynamik von polaren ZnO/MgZnO-Quantengraben(QW)-Strukturen zur exakten Bestimmung des unabgeschirmten Grundzustandes und der Analyse der zugrundeliegenden Emissionsprozesse. Dafür werden ausgehend von Beobachtungen an ZnO-Dünnschichten die Eigenschaften von mittels PLD hergestellten QWs unter dem Einfluss des internen elektrischen Feldes mit Hilfe der zeitintegrierten (TI-) und zeitaufgelösten (TR-) Photolumineszenz(PL)-Spektroskopie untersucht. Die Differenz der spontanen und piezoelektrischen Polarisation zwischen ZnO und MgZnO führt zur Ausbildung eines internen elektrischen Feldes und damit zum Auftreten des quantum-confined Stark effect (QCSE). Es wird gezeigt, dass der QCSE durch eine Durchmischung der Grenzflächen stark vermindert wird. Für QWs mit schwachem QCSE ist die Übergangsenergie und Zerfallszeit des Grundzustandes experimentell gut bestimmbar. Bei starkem QCSE müssen jedoch bereits bei geringen Anregungsdichten (1E10 /cm²) Abschirmeffekte berücksichtigt werden. Dadurch ist es sehr schwierig, den unabgeschirmten Grundzustand mittels herkömmlicher experimenteller Methoden mit einem aussagekräftigen Signal-Rausch-Verhältnis zu bestimmen. Es wird gezeigt, dass für QWs mit einer Dicke > 4 nm die Übergangsenergie des unabgeschirmten Grundzustandes nicht durch TI-PL-Messungen bestimmt werden kann. TR-PL-Messungen zeigen energetisch tiefere Übergangsenergien, jedoch ebenfalls nicht den unabgeschirmten Grundzustand. Mit einem eingeführten Modell zur Beschreibung der zeitabhängigen Abschirmung des Grundzustandsniveaus wird die Zerfallszeit für QW-Dicken in einem Bereich von 1 - 10 nm bestimmt. Durch die selbstkonsistente Lösung von Schrödinger- und Poissongleichung werden die Übergangsenergie und Zerfallszeit der Exzitonen im QW in Abhängigkeit der Feldstärke und auch der Ladungsträgerdichte berechnet. Dadurch ist eine exaktere Bestimmung der Feldstärke möglich. Zusätzlich wird durch die vergleichende Untersuchung von QWs unterschiedlicher Dicke, Potentialhöhe und Wachstumsunterlage die spontane und piezoelektrische Polarisation der Materialien experimentell bestimmt. Mittels temperaturabhängiger Messungen wird der Ursprung der Lumineszenz für QW-Dicken > 2 nm der Rekombination freier Exzitonen im QW zugeschrieben. Für dünnere QWs ist der temperaturabhängige Verlauf des PL-Maximums durch Lokalisation der Exzitonen bestimmt.

The construction of a high-resolution optical microscope system for micro-photoluminescence (µ-PL) spectroscopy is described, and a range of time-integrated and time-resolved experimental work on single InGaN quantum dots (QDs) is presented. Time-integrated measurements demonstrate the existence of InGaN QDs in three different samples via the presence of sharp exciton recombination lines in the µ-PL spectra. The narrowest peaks display a linewidth Γ of ~230 µeV, implying a decoherence time T2 ≥5.7 ps. Time-resolved measurements on exciton recombination lines from single self-assembled InGaN QDs reveal typical lifetimes of ~2.0 ns (which decrease with increasing temperature), while typical lifetimes for excitons in single selectively-grown micropyramidal InGaN QDs are found to be ~0.4 ns. The shorter exciton recombination lifetime in selectively-grown QDs is believed to be due to a stronger coupling of these QDs to the underlying quantum well. Temporal fluctuations (on a timescale of seconds) in the energy, intensity and FWHM of µ-PL peaks arising from the recombination of excitons in single self-assembled InGaN QDs are observed. These are attributed to transient Stark shifts induced by a fluctuating local charge distribution as carriers become trapped in defect states in the vicinity of the QDs. Time-integrated power-dependent measurements are used to demonstrate the presence of biexciton states in single self-assembled InGaN QDs. The exciton–biexciton energy splitting is found to be ~41 meV, in agreement with values predicted by theoretical calculations. Time-resolved studies of the biexciton and exciton decay curves reveal a coupling as the exciton population is refilled by biexciton decays. The biexciton lifetime is found to be ~1.4 ns, compared to an exciton lifetime of ~1.0 ns. Lateral electric fields are applied to a single self-assembled InGaN QD using aluminium electrodes lithographically defined on the sample surface. Application of fields of the order of ~0.17 MVcm-1 is found to cause both a red-shift and a reduction in the intensity of the exciton recombination peak in the µ-PL spectrum.

This thesis presents an investigation into the factors which control the gain and amplification properties in conjugated materials. Conjugated polymers and perylene dyes are highly fluorescent, are easy to process into thin films, and exhibit strong amplification over a broad gain bandwidth making them ideal for use in lasers and amplifiers. The stimulated emission created when thin films of the red emitting polymer poly(2-methoxy-5-(2'-ethylhexyloxy)- p-phenylenvinylene) (MEH-PPV) were photoexcited with high energy laser pulses was investigated. This was characterised by a dramatic narrowing of the emission spectrum which has been assigned to amplified spontaneous emission (ASE). The emission was found to have a gaussian profile and the gain coefficient was found to be 4 cm-1.The temperature dependence of the absorption, photoluminescence and ASE of films of MEH-PPV was measured. The effect of film morphology on the photophysical properties was investigated by using films cast from two spinning solvents, chlorobenzene (CB) and tetrahydrofuran (THE). Film morphology was found to greatly affect the temperature dependence. A particularly important property is the spectral position of the ASE and the factors which affect it. By controlling the film thickness close to the cut-off thickness for waveguiding in the polymer film it was shown that the peak position of the ASE could be tuned by 31 nm. Modelling of the waveguide modes in the polymer films was used to explain this effect. The cut-off wavelength for each film was measured and good agreement with the theory was found. In order to investigate ways in which energy transfer could be used to control the emission, two perylene dyes were used as a donor-acceptor pair in a host matrix of poly methymethacralate (PMMA). The position of the ASE was found to depend on the acceptor concentration. Measurements of the photoluminescence quantum yield and time-resolved luminescence measurements showed that the energy transfer coefficient was 5x10(^11)mol(^-1)d(^3)

No description available.

No description available.

This thesis contains primarily a study of CdTe/CdS heterojunction solar cells^ chiefly using photoluminescence spectroscopy. These solar cells show a good potential for commercial power generation in the near Aiture and are of interest to several major companies. A vital but little understood step in the manufacturing process is: annealing the cells in the presence of chlorine prior to back contact application. Studies are performed on a selection of thin film CdTe/CdS cells subjected to CdCl(_2) anneals of different duration. A chemical bevel etch was used to study the spectra at different depths into the sample and laser intensity arid sarhple temperature variations to identify the mechanisms behind the observed photoluminescence peaks. Evidence was found for the CdCl(_2) anneal promoting sulphur diffusion and subsequent grain boundary passivation in the CdTe, leading to increased minority carrier lifetimes and device efficiencies Attempts to obtain electroluminescence from the CdTe/CdS solar cells were madei By using current pulses electroluminescence was obtained in the 780-850nm range with discernible spectral features. Photoluminescence (PL) studies were also performed on a single crystal of CdTe grown to an unprecedented size of approx. 5 cm diameter at Durham university by a multi-tube seeded vapour method of crystal growth. Much higher resolution spectra were: obtained for this than for the solar cells. Several peaks were identified arid the mechanisms responsible were theorised. By taking slices of the crystal boule the PL spectra at different points-throughout the bulk of the crystal were determined. A series of high quality ion-implanted CdTe crystals were also studied! by intensity and temperature dependent PL in order to obtain a better understanding of the effects of known concentrations of known impurities on the PL spectra of CdTe. Specific PL features associated with certain dopants were observed.

In this study, we used ion implantation technique to synthesize semiconductor (Ge, Si) nanocrystals in SiO2 matrix. Ge and Si nanocrystals have been successfully formed by Ge and Si implantation and post annealing. Implanted samples were examined by characterization techniques such as TEM, XPS, EDS, SAD, SIMS, PL, Raman and FTIR spectroscopy and the presence of Ge and Si nanocrystals in the SiO2 matrix has been evidenced by these measurements. It was shown that implantation dose, implantation energy, annealing temperature, annealing time and annealing ambient are important parameters for the formation and evolution of semiconductor nanocrystals embedded in SiO2 matrix. The size and size distribution of Ge and Si nanocrystals were estimated successfully by fitting Raman and PL spectra obtained from Ge and Si implanted samples, respectively. It was demonstrated that Si implanted and post annealed samples exhibit two broad PL peaks at &amp / #8764 / 625 and 850 nm, even at room temperature. Origin of these peaks was investigated by temperature, excitation power and excitation wavelength dependence of PL spectrum and etch-measure experiments and it was shown that the peak observed at &amp / #8764 / 625 nm is related with defects (clusters or chain of Si located near the surface) while the other is related to the Si nanocrystals. As an expected effect of quantum size phenomenon, the peak observed at &amp / #8764 / 850 nm was found to depend on the nanocrystal size. Finally, the formation and evolution of Ge and Si nanocrystals were monitored by FTIR spectroscopy and it was shown that the deformation in SiO2 matrix caused by ion implantation tends to recover itself much quicker in the case of the Ge implantation. This is a result of effective segregation of Ge atoms at relatively low temperatures.

The results of photoluminescence (PL) spectra of TlGaS2 single crystal were reported in the 500-1400 nm wavelength and in the 15-115 K temperature range. Three broad PL bands with an asymmetric Gaussian lineshapes were observed to be centered at 568 nm (A-band), 718 nm (B-band) and 1102 nm (C-band). The shift of the emission band peak energy as well as the change of the half-width of the emission band with temperature and excitation laser intensity were also studied. We analyzed the observed results using the configurational coordinate (CC) model. The powder diffraction patterns of TlInS2 and TlGaS2 crystals were obtained and the diffraction data were indexed using CRYSFIRE computer program packet. TlInS2 has hexagonal system with parameters a = 3.83 and c = 14.88 Ao. TlGaS2 has monoclinic system with parameters a = 9.62, b = 4.01 and c = 7.52 Ao with &amp / #946 / = 96.30o. Our diffraction studies at low temperatures did not reveal any phase transition for TlInS2 as reported in the literature. The specific heat capacities of both TlInS2 and TlGaS2 crystals calculated from Differential Scanning Calorimetry (DSC) measurements at low temperatures are reported in the thesis.