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Disertacija skirta krūvininkų rekombinacijos tyrimams plačiatarpiuose nitridiniuose puslaidininkiuose bei jų dariniuose. Kompleksiniai eksperimentiniai tyrimai buvo atlikti naudojant kelias skirtingas metodikas. Atlikti krūvininkų dinamikos GaN sluoksniuose tyrimai labai žemų ir aukštų sužadinimų sąlygomis. Pasiūlytas naujas liuminescencijos gesimo kinetikų interpretavimo metodas, siejant liuminescencijos ir šviesa indukuotų dinaminių gardelių kinetikas. Naujas požiūris į geltonosios liuminescencijos juostą GaN sluoksniuose leido susieti geltonosios liuminescencijos intensyvumą su krūvininkų gyvavimo trukme. Skirtingomis technologijomis augintų AlGaN sluoksnių palyginimas suteikė informacijos apie juostos potencialo fliuktuacijas bei krūvininkų gyvavimo trukmę ribojančius veiksnius AlGaN medžiagose. Atskleista naujų krūvininkų dinamikos daugialakštėse AlGaN/AlGaN kvantinėse duobėse ypatumų – vidinio elektrinio lauko bei kvantinės duobės pločio fliuktuacijų sąlygotos lokalizacijos įtaka krūvininkų dinamikai. Dauguma tirtų bandinių buvo auginti naudojant MEMOCVDTM technologiją ir tyrimai patvirtino šios technologijos potencialą siekiant pagerinti medžiagų kokybę. / The thesis is dedicated to carrier recombination investigations in wide-band-gap semiconductors and their structures. The complex experimental studies were performed by combining several different techniques. Carrier dynamics in GaN epilayers were investigated under extremely low and high excitation conditions. A new method for interpreting photoluminescence decay kinetics was suggested by interrelating luminescence and light-induced grating decay transients. The new approach for studies of yellow band in GaN was shown by linking the carrier lifetime with yellow band intensity. Two AlGaN epilayers grown by different novel growth techniques were compared and the factors limiting carrier lifetime were identified. Moreover, more evidence on alloy mixing and band potential fluctuations in AlGaN was provided by our study. Essential knowledge was attained about carrier dynamics in high-Al-content AlGaN/AlGaN multiple quantum well structures: the influence of built-in electric field and carrier localization on carrier dynamics. Most of the samples under study were grown by MEMOCVDTM growth technique, and our study confirmed the high potential of this innovative growth technique for improving material quality.

The thesis is dedicated to carrier recombination investigations in wide-band-gap semiconductors and their structures. The complex experimental studies were performed by combining several different techniques. Carrier dynamics in GaN epilayers were investigated under extremely low and high excitation conditions. A new method for interpreting photoluminescence decay kinetics was suggested by interrelating luminescence and light-induced grating decay transients. The new approach for studies of yellow band in GaN was shown by linking the carrier lifetime with yellow band intensity. Two AlGaN epilayers grown by different novel growth techniques were compared and the factors limiting carrier lifetime were identified. Moreover, more evidence on alloy mixing and band potential fluctuations in AlGaN was provided by our study. Essential knowledge was attained about carrier dynamics in high-Al-content AlGaN/AlGaN multiple quantum well structures: the influence of built-in electric field and carrier localization on carrier dynamics. Most of the samples under study were grown by MEMOCVDTM growth technique, and our study confirmed the high potential of this innovative growth technique for improving material quality. / Disertacija skirta krūvininkų rekombinacijos tyrimams plačiatarpiuose nitridiniuose puslaidininkiuose bei jų dariniuose. Kompleksiniai eksperimentiniai tyrimai buvo atlikti naudojant kelias skirtingas metodikas. Atlikti krūvininkų dinamikos GaN sluoksniuose tyrimai labai žemų ir aukštų sužadinimų sąlygomis. Pasiūlytas naujas liuminescencijos gesimo kinetikų interpretavimo metodas, siejant liuminescencijos ir šviesa indukuotų dinaminių gardelių kinetikas. Naujas požiūris į geltonosios liuminescencijos juostą GaN sluoksniuose leido susieti geltonosios liuminescencijos intensyvumą su krūvininkų gyvavimo trukme. Skirtingomis technologijomis augintų AlGaN sluoksnių palyginimas suteikė informacijos apie juostos potencialo fliuktuacijas bei krūvininkų gyvavimo trukmę ribojančius veiksnius AlGaN medžiagose. Atskleista naujų krūvininkų dinamikos daugialakštėse AlGaN/AlGaN kvantinėse duobėse ypatumų – vidinio elektrinio lauko bei kvantinės duobės pločio fliuktuacijų sąlygotos lokalizacijos įtaka krūvininkų dinamikai. Dauguma tirtų bandinių buvo auginti naudojant MEMOCVDTM technologiją ir tyrimai patvirtino šios technologijos potencialą siekiant pagerinti medžiagų kokybę.

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Nitride-based semiconductor materials make it possible to fabricate optoelectronic devices that operate in the whole electromagnetic range, since the band gaps of these compounds can be modified by doping. Among these materials, the sp2-hybridized boron nitride has properties that make it a potential candidate for integration in devices operating in the short-wavelength limit, under harsh environment conditions, due to the strength of the B-N bond.  Nevertheless, this binary compound has been the less studied material among the nitrides, due to the lack of complete control on the growth process. This thesis is focused on the study of the optical properties of sp2-hybridized boron nitride grown by hot-wall chemical vapor deposition (CVD) method, at the Department of Physics, Chemistry and Biology, at Linköping University, Sweden. The samples received for this study were grown on c-plane aluminum nitride as the buffer layer, which in turn was grown by nitridation on c- plane oriented sapphire, as the substrate material. The first objective of the research presented in this thesis was the development of a suitable ellipsometry model in a spectral region ranging from the infrared to the ultraviolet zones of the electromagnetic spectrum, with the aim of obtaining in the process optical properties such as the index of refraction, the energy of the fundamental electronic interband transition, the frequencies for the optical vibrational modes of the crystal lattice, as well as their broadenings, and the numerical values of the dielectric constants; and on the other hand, structural parameters such as the layers thicknesses, and examine the possibility of the presence of roughness or porosity on the boron nitride layer, which may affect the optical properties, by incorporating their effects into the model. The determination of these parameters, and their relation with the growth process, is important for the future adequate design of heterostructure-based devices that incorporate this material. In particular, emphasis has been put on the modeling of the polar lattice resonance contributions, with the TO- LO model, by using infrared spectroscopic ellipsometry as the characterization technique to study the phonon behavior, in the aforementioned spectral region, of the boron nitride. On the other hand, spectroscopic ellipsometry in the visible-ultraviolet spectral range was used to study the behavior of the material, by combining a Cauchy model, including an Urbach tail for the absorption edge, and a Lorentz oscillator in order to account for the absorption in the material in the UV zone. This first step on the research project was carried out at Linköping University.  The second objective in the research project was to carry out additional studies on the samples received, in order to complement the information provided by the ellipsometry model and to improve the model itself, provided that it was possible. The characterization techniques used were X-ray diffraction, which made it possible to confirm that in fact boron nitride was present in the samples studied, and made it possible to verify the crystalline quality of the aforementioned samples, and in turn relate it to the quality of the ellipsometry spectra previously obtained; the Raman spectroscopy made it possible to further verify and compare the crystalline qualities of the samples received, as well as to obtain the frequency for the Raman active B-N stretching vibration in the basal plane, and to compare this value with that corresponding to the bulk sp2-boron nitride; scanning electron microscopy made it possible to observe the rough surface morphologies of the samples and thus relate them to some of the conclusions derived from the ellipsometry model; and finally cathodoluminescence measurements carried out at low temperature (4 K) allowed to obtain a broad band emission, on all the samples studied, which could be related to native defects inside the boron nitride layers, i.e., boron vacancies. Nevertheless, no trace of a free carrier recombination was observed. Considering that the hexagonal-boron nitride is nowadays considered to be a direct band gap semiconductor, it may be indirectly concluded, in principle, that the dominant phase present in the samples studied was the rhombohedral polytype. Moreover, it can be tentatively concluded that the lack of an observable interband recombination may be due to the indirect band gap nature of the rhombohedral phase of the boron nitride. Spectroscopic ellipsometry does not give a definite answer regarding this issue either, because the samples analyzed were crystalline by nature, thus not being possible to use mathematical expressions for the dielectric function models that incorporate the band gap value as a fitting parameter. Therefore, the nature of the band gap emission in the rhombohedral phase of the boron nitride is still an open research question. On the other hand, luminescent emissions originating from radiative excitonic recombinations were not observed in the cathodoluminescence spectra. This second step of the project was carried out at the Leroy Eyring Center for Solid State Science at Arizona State University.

The thesis is dedicated to investigation of carrier dynamics in InN, InGaN, and GaAsBi heterostructures by using light-induced transient gratings and differential transmission techniques. The experimental studies in a wide range of excess carrier densities and temperatures revealed that trap-assisted Auger recombination is the dominant recombination mechanism in MBE-grown InN layers at room temperature. Investigation of carrier dynamics in In-rich InGaN alloys revealed that density of fast nonradiative recombination centers increases with Ga content. The correlation between excess carrier lifetime and diffusion coefficient in MOCVD-grown single InGaN layer with 13% In is governed by diffusive flow to the extended defects. Investigations of carrier lifetime and diffusivity dependence on excitation fluence indicated that both nonradiative and radiative recombination contribute to an increase of excess carrier recombination rate at high photo-excitation levels in MOCVD-grown InGaN multiple quantum wells. Transient grating measurements in MBE-grown GaAsBi layers with different Bi content revealed that Bi induced potential fluctuations determine the tenfold decrease in nonequilibrium hole mobility, if compare to GaAs. / Disertacija skirta nepusiausvirųjų krūvininkų dinamikos tyrimams InN, InGaN ir GaAsBi heterosandarose naudojant šviesa indukuotų dinaminių gardelių ir skirtuminio pralaidumo metodikas. Atlikti tyrimai plačiame nepusiausvirųjų krūvininkų tankių ir bandinio temperatūrų intervale parodė, kad krūvininkų rekombinacijos sparta MBE būdu užaugintuose InN sluoksniuose dominuojantis rekombinacijos mechanizmas kambario temperatūroje yra gaudyklių įtakota Ožė rekombinacija. Nustatyta koreliacija tarp krūvininkų gyvavimo trukmės ir difuzijos koeficiento MOCVD būdu užaugintame InGaN sluoksnyje su 13% In parodė, kad krūvininkų gyvavimo trukmę lemia difuzinė jų perneša link rekobinacijos centrų. Parodoma, kad MBE metodu užaugintuose InGaN sluoksniuose su dideliu In kiekiu (x>0,7) didėjant Ga kiekiui didėja nespindulinės rekombinacijos centrų tankis, o krūvininkų rekombinacijos sparta yra termiškai aktyvuojama. MOCVD metodu užaugintose InGaN kvantinėse sandarose dinaminių gardelių tyrimais parodoma, kad spartėjančią krūvininkų rekombinaciją didėjant sužadinimo intensyvumui lemia ne tik spindulinė rekombinacija, tačiau reikia atsižvelgti ir į nespindulinės rekombinacijos spartėjimą. Nustatyta, kad į GaAs įterpiant Bi atomus daugiau nei dešimt kartų sumažėja skylių judris dėl Bi atomų kuriamų valentinės juostos fliuktuacijų.

Disertacija skirta nepusiausvirųjų krūvininkų dinamikos tyrimams InN, InGaN ir GaAsBi heterosandarose naudojant šviesa indukuotų dinaminių gardelių ir skirtuminio pralaidumo metodikas. Atlikti tyrimai plačiame nepusiausvirųjų krūvininkų tankių ir bandinio temperatūrų intervale parodė, kad krūvininkų rekombinacijos sparta MBE būdu užaugintuose InN sluoksniuose dominuojantis rekombinacijos mechanizmas kambario temperatūroje yra gaudyklių įtakota Ožė rekombinacija. Nustatyta koreliacija tarp krūvininkų gyvavimo trukmės ir difuzijos koeficiento MOCVD būdu užaugintame InGaN sluoksnyje su 13% In parodė, kad krūvininkų gyvavimo trukmę lemia difuzinė jų perneša link rekobinacijos centrų. Parodoma, kad MBE metodu užaugintuose InGaN sluoksniuose su dideliu In kiekiu (x>0,7) didėjant Ga kiekiui didėja nespindulinės rekombinacijos centrų tankis, o krūvininkų rekombinacijos sparta yra termiškai aktyvuojama. MOCVD metodu užaugintose InGaN kvantinėse sandarose dinaminių gardelių tyrimais parodoma, kad spartėjančią krūvininkų rekombinaciją didėjant sužadinimo intensyvumui lemia ne tik spindulinė rekombinacija, tačiau reikia atsižvelgti ir į nespindulinės rekombinacijos spartėjimą. Nustatyta, kad į GaAs įterpiant Bi atomus daugiau nei dešimt kartų sumažėja skylių judris dėl Bi atomų kuriamų valentinės juostos fliuktuacijų. / The thesis is dedicated to investigation of carrier dynamics in InN, InGaN, and GaAsBi heterostructures by using light-induced transient gratings and differential transmission techniques. The experimental studies in a wide range of excess carrier densities and temperatures revealed that trap-assisted Auger recombination is the dominant recombination mechanism in MBE-grown InN layers at room temperature. Investigation of carrier dynamics in In-rich InGaN alloys revealed that density of fast nonradiative recombination centers increases with Ga content. The correlation between excess carrier lifetime and diffusion coefficient in MOCVD-grown single InGaN layer with 13% In is governed by diffusive flow to the extended defects. Investigations of carrier lifetime and diffusivity dependence on excitation fluence indicated that both nonradiative and radiative recombination contribute to an increase of excess carrier recombination rate at high photo-excitation levels in MOCVD-grown InGaN multiple quantum wells. Transient grating measurements in MBE-grown GaAsBi layers with different Bi content revealed that Bi induced potential fluctuations determine the tenfold decrease in nonequilibrium hole mobility, if compare to GaAs.

Ce travail de thèse porte sur la croissance par épitaxie par jets moléculaires assistée plasma et sur la caractérisation de nanofils (NF) de GaN et d'hétérostructures filaires de GaN/AlN. Dans un premier temps, la morphologie des NFs de GaN (densité, longueur moyenne, diamètre moyen, dispersion de longueurs) est étudiée en fonction des paramètres de croissance. Via la diffraction d'électrons rapides, la morphologie des NFs GaN est corrélée à la dynamique de nucléation de ces derniers. Des expériences de diffraction de rayons X en incidence rasante effectuées à l'ESRF permettent également de clarifier les processus de nucléation des NFs GaN. Nous démontrons ensuite l'utilisation de la diffraction de rayons X résonnante pour déterminer la polarité des NFs GaN. Nous montrons que ces derniers sont de polarité N lorsque fabriqués sur Si nu. Des tests complémentaires de gravure sélective au KOH révèlent que les NFs GaN fabriqués sur un substrat de Si recouvert d'un fin buffer d'AlN ainsi que ceux dont la fabrication est initiée après pré-déposition de Ga sur la surface du Si, sont aussi de polarité N. Concernant les hétérostructures filaires GaN-AlN, la croissance d'AlN autour et sur les nanofils de GaN est étudiée en fonction de divers paramètres de croissance. Le rapport d'aspect des coquilles d'AlN (longueur/épaisseur) est décrit par un modèle géométrique. En utilisant une combinaison de diffraction anomale multi-longueurs d'onde, de microscopie en transmission de haute résolution et des calculs théoriques, l'état de contrainte des coeurs de GaN est analysé en fonction de l'épaisseur de la coquille. Cette contrainte augmente avec l'épaisseur de la coquille tant que l'AlN croît de manière homogène autour des NFs de GaN. Dès lors que la coquille est asymétrique, le système relaxe plastiquement. Nous étudions enfin la possibilité de fabriquer des îlots de GaN dans des NFs AlN. Nous déterminons le rayon critique de NFs AlN au-dessus duquel le GaN déposé subit une transition de forme de 2D à 3D. L'analyse des propriétés optiques de ces nanostructures originales revèle la présence de nombreux états localisés. / This work focuses on the growth by plasma-assisted molecular beam epitaxy and on the characterization of GaN nanowires (NWs) and of GaN/AlN NW heterostructures. We first investigate GaN NW morphology (density, mean length, mean diameter, length dispersion) dependence on the growth parameters. Using reflection high energy electron diffraction, GaN NW morphology is correlated to their nucleation dynamics. In situ grazing-incidence X-ray diffraction experiments performed at the ESRF allow clarifying GaN NW nucleation processes on bare Si(111) and when usinga thin AlN buffer deposited on Si(111). The use of resonant X-ray diffraction for the determination of GaN NW polarity is then successfully demonstrated. GaN NWs grown on bare Si(111) are shown to be N-polar. Additional KOH selective etching tests reveal that both GaN NWs grown using a thin AlN buffer on Si(111) and when pre-depositing Ga on the Si(111) surface are N-polar, too. Regarding GaN-AlN NW heterostructures, the growth of an AlN shell around GaN NWs is studied as a function of various growth parameters. The AlN shell aspect ratio is described by a geometrical model. Using a combination of multiwavelength anomalous diffraction, high resolution transmission microscopy and theoretical calculations, GaN core strain state is investigated as a function of the AlN shell thickness. This strain is shown to increase with the shell thickness as long as AlN grows homogeneously around GaN NWs. When the shell is asymmetric, the system relaxes plastically. Eventually, we study the possibility to fabricate island-like GaN insertions in AlN NWs. We determine the critical AlN NW radius above which GaN undergoes a 2D to 3D shape-transition. Regarding optical properties of these novel structures, the presence of multiple localized states is identified.

Surface structure, chemical composition, bonding configuration, film polarity, and electronic properties of InN layers grown by high pressure chemical vapor deposition (HPCVD) have been investigated. Sputtering at an angle of 50-70 degrees followed by atomic hydrogen cleaning (AHC) was successful in removing the carbon contaminants. AHC is found to be the most effective cleaning process to remove oxygen contaminants from InN layers in an ultrahigh vacuum (UHV) system and produced a well ordered surface. Auger electron spectroscopy (AES) confirmed the cleanliness of the surface, and low energy electron diffraction (LEED) yielded a 1×1 hexagonal pattern demonstrating a well-ordered surface. High resolution electron energy loss spectra (HREELS) taken from the InN layers exhibited loss features at 550 cm-1, 870 cm-1 and 3260 cm-1 which were assigned to Fuchs-Kliewer phonon, N-H bending, and N-H stretching vibrations, respectively. Assignments were confirmed by observation of isotopic shifts following atomic deuterium dosing. No In-H species were observed indicating N-termination of the surface and N-polarity of the film. Broad conduction band plasmon excitations were observed centered at 3100 cm-1 to 4200 cm-1 in HREEL spectra acquired with 25 eV electrons, for a variety of samples grown with different conditions. Infrared reflectance data shows a consistent result with HREELS for the bulk plasma frequency. The plasmon excitations are shifted about 300 cm-1 higher in HREEL spectra acquired using 7 eV electrons due to the higher plasma frequency and carrier concentration at the surface than in the bulk, demonstrating a surface electron accumulation. Hydrogen completely desorbed from the InN surface upon annealing for 900 s at 425 ºC or upon annealing for 30 s at 500 ºC. Fitting the coverage versus temperature for anneals of either 30 or 900 s indicated that the desorption was best described by second order desorption kinetics with an activation energy and pre-exponential factor of 1.3±0.2 eV and 10-7.3±1.0 cm2/s, respectively. Vibrational spectra acquired from HREEL can be utilized to explain the surface composition, chemical bonding and surface termination, and film polarity of InN layers. The explanation of evidence of surface electron accumulation and extraction of hydrogen desorption kinetic parameters can be performed by utilizing HREEL spectra.

Thesis (M.App.Sc.) - Carleton University, 2007. / Includes bibliographical references (p. 73-76). Also available in electronic format on the Internet.