Thesis (M.S.)--Ohio University, June, 2005. / Includes bibliographical references (p. 46-50)

Thesis (Ph. D.)--University of Washington, 2005. / Vita. Includes bibliographical references (leaves 106-116).

Thesis (M.S.)--Ohio University, June, 2005. / Title from PDF t.p. Includes bibliographical references (p. 46-50)

Deep ultraviolet (UV) light sources are useful in a number of applications that include sterilization, medical diagnostics, as well as chemical and biological identification. However, state-of-the-art deep UV light-emitting diodes and lasers made from semiconductors still suffer from low external quantum efficiency and low output powers. These limitations make them costly and ineffective in a wide range of applications. Deep UV sources such as lasers that currently exist are prohibitively bulky, complicated, and expensive. This is typically because they are constituted of an assemblage of two to three other lasers in tandem to facilitate sequential harmonic generation that ultimately results in the desired deep UV wavelength. For semiconductor-based deep UV sources, the most challenging difficulty has been finding ways to optimally dope the (Al,Ga)N/GaN heterostructures essential for UV-C light sources. It has proven to be very difficult to achieve high free carrier concentrations and low resistivities in high-aluminum-containing III-nitrides. As a result, p-type doped aluminum-free III-nitrides are employed as the p-type contact layers in UV light-emitting diode structures. However, because of impedance-mismatch issues, light extraction from the device and consequently the overall external quantum efficiency is drastically reduced. This problem is compounded with high losses and low gain when one tries to make UV nitride lasers. In this thesis, we provide a robust and reproducible approach to resolving most of these challenges. By using a liquid-metal-enabled growth mode in a plasma-assisted molecular beam epitaxy process, we show that highly-doped aluminum containing III-nitride films can be achieved. This growth mode is driven by kinetics. Using this approach, we have been able to achieve extremely high p-type and n-type doping in (Al,Ga)N films with high aluminum content. By incorporating a very high density of Mg atoms in (Al,Ga)N films, we have been able to show, by temperature-dependent photoluminescence, that the activation energy of the acceptors is substantially lower, thus allowing a higher hole concentration than usual to be available for conduction. It is believed that the lower activation energy is a result of an impurity band tail induced by the high Mg concentration. The successful p-type doping of high aluminum-content (Al,Ga)N has allowed us to demonstrate operation of deep ultraviolet LEDs emitting at 274 nm. This achievement paves the way for making lasers that emit in the UV-C region of the spectrum. In this thesis, we performed preliminary work on using our structures to make UV-C lasers based on photonic crystal nanocavity structures. The nanocavity laser structures show that the threshold optical pumping power necessary to reach lasing is much lower than in conventional edge-emitting lasers. Furthermore, the photonic crystal nanocavity structure has a small mode volume and does not need mirrors for optical feedback. These advantages significantly reduce material loss and eliminate mirror loss. This structure therefore potentially opens the door to achieving efficient and compact lasers in the UV-C region of the spectrum.

Ce travail de thèse porte sur la croissance et sur la caractérisation optique de nanostructures à base d’antimoine sur substrats InP, en vue d’applications dans le domaine des télécommunications optiques. La transition inter-sous-bande est un processus ultrarapide qui permet la modulation de la lumière dans les réseaux de télécommunication optique. Durant cette thèse, une absorption inter-sous-bande dans le proche-infrarouge provenant de puits quantiques Ga0.47In0.53As/AlAs0.56Sb0.44 a été observée pour la première fois au laboratoire. Les analyses par microscopie électronique à effet tunnel sur la face clivée montrent cependant de nombreux déviations à l’idéalité de nos structures : mélange à l’échelle atomique aux interfaces entre GaInAs et AlAsSb, inhomogénéité de l’alliage GaInAs, incorporation non-intentionnel d’antimoine dans le GaInAs. Les puits quantiques InAs/AlAs0.56Sb0.44 sont potentiellement des objets de choix pour la réalisation de composants intersous- bande travaillant à 1,55 μm. Des puits quantiques InAs/AlAs0.56Sb0.44 contraint, exempt de défauts ont été obtenus par croissance assistée par effet surfactant de Sb. En symétrisant la contrainte induite par le dépôt d’InAs par l’insertion de couches nanométriques de AlAs dans les barrières, des multi-puits InAs/AlAs0.56Sb0.44 sans contrainte macroscopique ont été réalisés. L’effet de l’antimoine en surface sur la croissance de structure InAs/GaAs0.51Sb0.49 a également été étudié. En présence d’antimoine sur substrats InP d’orientation (001), le dépôt d’InAs conduit à la formation de puits quantiques. Par contre sur ceux orientés suivant (113)B des boites quantiques sont formées suivant le mode de croissance Volmer-Weber. Ces résultats sont discutés en termes d’effets cinétiques ou énergétiques de l’antimoine en surface. La modification de l’anisotropie de l’énergie de surface induite par l’antimoine permet d’interpréter nos résultats sur substrats (100) et (113) B. / This PhD work presents molecular beam epitaxy growth and optical studies on several Sb-nanostructures on InP substrate, for their potential use in optical telecommunication. Inter-subband transition in Ga0.47In0.53As/AlAs0.56Sb0.44 quantum well is a useful physical process for implementing ultrafast fulloptical modulations. Near-infrared inter-subband transition in this material was achieved and microscopic studies on this structure has revealed that the intermixing at GaInAs/AlAsSb interface, unintentional Sb incorporation in GaInAs layer and the inhomogeneity within GaInAs layer could prevent Ga0.47In0.53As/ AlAs0.56Sb0.44 multiple quantum wells from achieving intersubband transition in 1.55 μm optical telecommunication band. The strained InAs/AlAs0.56Sb0.44 quantum well is another material that has potential use in 1.55 μm full-optical modulation. 2 nm-thick defect-free InAs/AlAs0.56Sb0.44 was obtained under Sb surfactant-mediated growth, and by using strain compensation techniques, InAs/AlAs0.56Sb0.44 multiple quantum wells with zero net-strain were realized. The study of Sb-mediated growth is also carried on to InAs/GaAs0.51Sb0.49 nanostructures. The growths of such structures on InP (001) substrate has led to the formation of flat InAs layer, while high-density InAs/GaAs0.51Sb0.49 quantum dots were obtained on InP (113)B substrates under Volmer-Weber growth mode. We attribute such phenomena to the surfaceorientation dependent surfactant effect of Sb. Emission wavelength close to 2 μm was achieved with only 5 ML of InAs deposition, which makes these quantum dots attractive to InPbased mid-wave applications.

Deep ultraviolet light emitting diodes (UV LEDs) are an important emerging technology for a number of applications such as water/air/surface disinfection, communications, and epoxy curing. However, as of yet, deep UV LEDs grown on sapphire substrates are neither efficient enough nor powerful enough to fully serve these and other potential applications. The majority of UV LEDs reported so far in the literature are grown on sapphire substrates and their design consists of AlGaN quantum wells (QWs) embedded in an AlGaN p-i-n junction with the n-type layer on the sapphire. These devices suffer from a high concentration of threading defects originating from the large lattice mismatch between the sapphire substrate and AlGaN alloys. Other issues include the poor doping efficiency of the n- and particularly the p-AlGaN alloys, the extraction of light through the sapphire substrate, and the heat dissipation through the thermally insulating sapphire substrate. These problems have historically limited the internal quantum efficiency (IQE), injection efficiency (IE), and light extraction efficiency (EE) of devices. As a means of addressing these efficiency and power challenges, I have contributed to the development of a novel inverted vertical deep UV LED design based on AlGaN grown on p-SiC substrates. Starting with a p-SiC substrate that serves as the p-type side of the p-i-n junction largely eliminates the necessity for the notoriously difficult p-type doping of AlGaN alloys, and allows for efficient heat dissipation through the highly thermally conductive SiC substrate. UV light absorption in the SiC substrate can be addressed by first growing p-type doped distributed Bragg reflectors (DBRs) on top of the substrate prior to the deposition of the active region of the device. A number of n-AlGaN films, AlGaN/AlGaN multiple quantum wells, and p-type doped AlGaN DBRs were grown by molecular beam epitaxy (MBE). These were characterized in situ by reflected high energy electron diffraction (RHEED) and ex situ by x-ray diffraction, scanning electron microscopy, atomic force microscopy, photoluminescence, and reflectivity. Using the primary elements of the proposed design, this research culminated in the MBE growth, fabrication, and characterization of prototype deep UV LED devices emitting below 300 nm.

<p></p><p>High mobility 2DEG (two-dimensional electron gas) confined in GaAs is a good platform to understand correlated electron systems and a promising candidate for qubit devices. For example, the non-Abelian feature of Fractional Quantum Hall state enabling topological quantum computation is only found in GaAs with high mobility. Theoretical calculations have shown that the mobility is inversely proportional to impurities in GaAs/AlGaAs heterstructures grown by Molecular Beam Epitaxy (MBE). In recent MBE experiments, the source Ga was found to be more important in the limitation of mobility than Al and As. A high mobility of 35 million cm²/Vs was recently observed when an 8N Ga (total nominal impurity concentration of ~10 ppb) source was used compared to 25 million cm²/Vs for a 7N Ga source. In addition, significant mobility increase was observed after in-situ distillation of the source Ga before growth. In order to clarify the mechanism of how the distillation contributed to the Ga purification, thus resulting in the mobility increase, the MBE in-situ distillation was analyzed by molecular distillation theory. Evaporation behavior of solvent Ga was analyzed including effects of evaporation from a crucible with receding liquid depth. Then impurity removal through molecular distillation was analyzed with molecular evaporation kinetics. The remaining 7N and 8N Ga after in-situ MBE distillation and growth were elementally analyzed by ICP-MS (Inductively Coupled Plasma Mass Spectrometry) and compared with analyses of the starting 7N and 8N Ga from same lots. Due to the increased detection limit of ICP-MS in metal analysis, the concentrations of most impurity elements reached the detection limit of ~1-10 ppb. However, unusual high concentration of 690 ppb Ge was found in the 7N Ga, exceeding the nominal concentration of 7N (100 ppb). Significant decrease in Ge concentration was found in the comparison of initial ultra-pure Ga and remaining Ga for both grades of 7N and 8N. The significant Ge losses cannot be explained by atomic Ge evaporation due to the low vapor pressure of Ge. However, a hypothesis of Ge evaporation as GeO(g) by Ge active oxidation was proposed. In order to test the active oxidation of very dilute Ge in Ga in the MBE conditions with very low P(O₂), the equilibrium P(GeO)-P(O₂) vapor species diagram was calculated from thermodynamics. The analysis shows that even very dilute Ge in Ga of ~ 1 ppm concentration can be <a>actively oxidized in the extremely low P(O₂) of MBE</a>. In order to prove active oxidation of Ge, molecular distillation of 7N Ga was performed in <a>a specially constructed high vacuum chamber. The 7N Ga with unusual high Ge concentration of 440 ppb (by GDMS analysis) was distilled for 16 h at 1360 K under the starting P(O₂) of 3 x 10^-6 torr and the total pressure of 10^-5 torr. The chamber vacuum was monitored by Residual Gas Analyzer (RGA) and the residual Ga after 16 h distillation was analyzed by GDMS. In the GDMS analysis, significant Ge loss was found from 440 ppb to below the detection limit of 10 ppb, confirming Ge active oxidation hypothesis. The oxygen-assisted impurity removal in distillation also may be applicable to other impurities with high vapor pressure gaseous oxide, but low vapor pressure itself, such as Al, Si and Sn. </a></p><br><p></p>

Group III-nitride materials have attracted great attention for applications in high efficiency electronic and optoelectronics devices such as high electron mobility transistors, light emitting diodes, and laser diodes. On the other hand, group VI transition metal dichalcogenides (TMDs) in the form of MX2 has recently emerged as a novel atomic layered material system with excellent thermoelectric, electronic and optoelectronic properties. Also, the recent investigations reveal that the dissimilar heterojunctions formed by TMDs and III-nitrides provide the route for novel devices in the area of optoelectronic, electronics, and water splitting applications. In addition, integration of III-nitrides and TMDs will enable high density integrated optoelectronic circuits and the development of hybrid integration technologies. In this work, we have demonstrated kinetically controlled growth processes in plasma assisted molecular beam epitaxy (PAMBE) for the III-nitrides and their engineered heterostructures. Techniques such as Ga irradiation and nitrogen plasma exposure has been utilized to implement bulk GaN, InGaN and their heterostructures in PAMBE. For the growth of III-nitride based heterostructures, the in-situ surface stoichiometry monitoring (i-SSM) technique was developed and used for implementing stepped and compositionally graded InGaN-based multiple quantum wells (MQWs). Their optical and microstrain analysis in conjunction with theoretical studies confirmed improvement in the radiative recombination rate of the graded-MQWs as compared to that of stepped-MQWs, owing to the reduced strain in graded-MQWs. Our achievement also includes the realization of the p-type MoS2 by engineering pristine MoS2 layers in PAMBE. Mainly, Ga and nitrogen plasma irradiation on the pristine MoS2 in PAMBE has resulted in the realization of the p-type MoS2. Also, GaN epitaxial thin layers were deposited on MoS2/c-sapphire, WSe2/c-sapphire substrates by PAMBE to study the band discontinuity at GaN/TMDs heterointerface. The determination of band offset parameters for both GaN/MoS2 and GaN/WSe2 heterostructures revealed realization of type-II band alignment. Also, heterojunctions such as AlGaN/MoS2 is implemented to achieve type-I heterojunction. This work may open up a new avenue towards photonic quantum devices based on the integration of III-nitrides with 2D TMDs.

No description available.

Self-catalyzed GaAs nanowires (NWs) are grown epitaxially on Si(111) substrates using molecular beam epitaxy (MBE). The dynamics of the droplet are examined to improve NW yield and to control NW morphology. Control and understanding of the NW diameter via droplet dynamics is applied to NW photovoltaics and to novel corrugated NW distributed Bragg reflectors (DBRs). At the beginning of the MBE growth, a Ga pre-deposition step, between 0 s and 500 s in duration, is introduced to improve the yield of the NW arrays. The effect of the pre-deposition time was examined for five different hole diameters and yield was increased to nearly 100% for the appropriate combination of hole diameter and pre-deposition time. Two models were used to model the NW growth progression under different atomic flux ratios. The first model considers the contributions from direct and diffusion fluxes to the droplet and solves coupled equations for the droplet contact angle and the NW radius. The second model treats the contact angle as constant. Both models explained the accompanying experimental observations. Both models could be used to model future NW growths and the choice between the two would depend on the availability of contact angle data and whether the crystal phase must be considered. Absorption in NWs is determined by the diameter and the HE1n modes. The effectiveness of a linearly tapered inverted conical NW is demonstrated using finite element simulations. The photocurrent of an optimized inverted conical NW array is found and shown to be similar to that achieved by optical nanocones and nanowires. Diameter modulations can also be introduced into NW structures periodically to produce corrugated NW distributed Bragg reflectors (DBRs). The tunability of the reflectance peaks is demonstrated and explained by changes to the effective refractive index of the structure. / Thesis / Doctor of Philosophy (PhD) / This thesis seeks to understand the growth processes behind self-catalyzed nanowire growth. Nanowires (NWs) are very thin, vertical columns of semiconducting material. Self-catalyzed growth is a method of producing these structures that uses a droplet at the top of the structure to add material to the structure over time. These structures have numerous applications. This thesis focuses on solar cells and distributed Bragg reflectors (DBRs). Experiments show how control over the droplet can improve NW yield and give significant control of the NW diameter. These experiments are supported by mathematical models. Control over the diameter is important for the applications discussed. Using numerical simulations, it is shown how control over the diameter of the structure can lead to improvements in light absorption in NW solar cells. Additionally, periodic changes to the diameter can be used to create novel NW structures such as DBRs, which is a promising new application.