Thesis (Ph. D.)--Ohio University, March, 2000. / Title from PDF t.p.

The popularity of III-nitride materials has taken up the semiconductor industry to newer applications because of their remarkable properties. In addition to having a direct and wide band gap of 3.4 eV, a very fascinating property of GaN is the band gap tuning from 0.7 to 6.2 eV by alloying with Al or In. The most common orientation to grow optoelectronic devices out of these materials are the polar c-plane which are strongly affected by the intrinsic spontaneous and piezoelectric polarization fields. Devices grown in no polar orientation such as (1 0 –1 0) m-plane or (1 1 –2 0) a-plane have no polarization in the growth direction and are receiving a lot of focus due to enhanced behaviour. The first part of this thesis deals with the development of non-polar epimGaN films of usable quality, on an m-plane sapphire by plasma assisted molecular beam epitaxy. Growth conditions such as growth temperature and Ga/N flux ratio were tuned to obtain a reasonably good crystalline quality film. MSM photodetectors were fabricated from (1 0 -1 0) m-GaN, (1 1 -2 0) a-GaN and semipolar (1 1 -2 2) GaN films and were compared with the polar (0 0 0 2) c-GaN epilayer. Later part of the thesis investigated (1 0 -1 0) InN/ (1 0 -1 0) GaN heterostructures. Further, we could successfully grow single composition nonpolar a-plane InxGa1-xN epilayers on (1 1 -2 0) GaN / (1 -1 0 2) sapphire substrate. This thesis focuses on the growth and characterisation of nonpolar GaN, InxGa1-xN and InN by plasma assisted molecular beam epitaxy and on their photodetection potential. Chapter 1 explains the motivation of this thesis work with an introduction to the III-nitride material and the choice of the substrate made. Polarization effect in the polar, nonpolar and semipolar oriented growth is discussed. Fabrication of semiconductor photodetectors and its principle is explained in details. Chapter 2 discusses the various experimental tools used for the growth and characterisation of the film. Molecular beam epitaxy technique is elaborately explained along with details of the calibration for the BEP of various effusion cells along with growth temperature at the substrate. Chapter 3 discusses the consequence of nitridation on bare m-sapphire substrate. Impact of nitridation step prior to the growth of GaN film over (1 0 -1 0) m-sapphire substrate was also studied. The films grown on the nitridated surface resulted in a nonpolar (1 0 -1 0) orientation while without nitridation caused a semipolar (1 1 -2 2) orientation. Room temperature photoluminescence study showed that nonpolar GaN films have higher value of compressive strain as compared to semipolar GaN films, which was further confirmed by room temperature Raman spectroscopy. The room temperature UV photodetection of both films was investigated by measuring the I-V characteristics under UV light illumination. UV photodetectors fabricated on nonpolar GaN showed better characteristics, including higher external quantum efficiency, compared to photodetectors fabricated on semipolar GaN. Chapter 4 focuses on the optimization and characterisation of nonpolar (1 0 -1 0) m-GaN on m-sapphire by molecular beam epitaxy. A brief introduction to the challenges in growing a pure single phase nonpolar (1 0 -1 0) GaN on (1 0 -1 0) sapphire without any other semipolar GaN growth is followed by our results achieving the same. Effect of the growth temperature and Ga/N ratio on the structural and optical properties of m-GaN epilayers was studied and the best condition was obtained for the growth temperature of 7600C and nitrogen flow of 1 sccm. Strain in the film was quantitatively measured using Raman spectroscopy and qualitatively analyzed by RSM. Au/ nonpolar GaN schottky diode was fabricated and temperature dependent I-V characteristics showed rectifying nature. Chapter 5 demonstrates the growth of (1 0 -1 0) m-InN / (1 0 -1 0) m-GaN / (1 0 -1 0) m-sapphire substrate. Nonpolar InN layer was grown at growth temperature ranging from 3900C to 440C to obtain a good quality film at 4000C. An in-plane relationship was established for the hetrostructures using phi-scan and a perfect alignment was found for the epilayers. RSM images on the asymmetric plane revealed highly strained layers. InN band gap was found to be around 0.8 eV from absorption spectra. The valance band offset value is calculated to be 0.93 eV for nonpolar m-plane InN/GaN heterojunctions. The heterojunctions form in the type-I straddling configuration with a conduction band offsets of 1.82 eV. Chapter 6 focuses on the optimization of nonpolar (1 1 -2 0) a-GaN on (1 -1 0 2) r-sapphire by molecular beam epitaxy. Effect of the growth temperature and Ga/N ratio on the structural and optical properties of a-GaN epilayers was studied and the best condition was obtained for the growth temperature of 7600C and nitrogen flow of 1 sccm. An in-plane orientation relationship is found to be [0 0 0 1] GaN || [-1 1 0 1] sapphire and [-1 1 0 0] GaN || [1 1 -2 0] sapphire for nonpolar GaN on r-sapphire substrate. Strain in the film was quantitatively measured using Raman spectroscopy and qualitatively analyzed by RSM. UV photo response of a-GaN film was measured after fabricating an MSM structure over the film with Au. EQE of the photodetectors fabricated in the (0 0 0 2) polar and (1 1 -2 0) nonpolar growth directions were compared in terms of responsively, nonpolar a-GaN showed the best sensitivity at the cost of comparatively slow response time. Chapter 7 demonstrates the growth of non-polar (1 1 -2 0) a-plane InGaN epilayers on a-plane (1 1 -2 0) GaN/ (1 -1 0 2) r-plane sapphire substrate using PAMBE. The high resolution X-ray diffraction (HRXRD) studies confirmed the orientation of the films and the compositions to be In0.19Ga0.81N, In0.21Ga0.79N and In0.23Ga0.77N. The compositions of the films were controlled by the growth parameters such as growth temperature and indium flux. Effect of variation of Indium composition on the strain of the epilayers was analyzed from the asymmetric RSM images. Further, we report the growth of self-assembled non-polar high indium clusters of In0.55Ga0.45N over non-polar (1 1 -2 0) a-plane In0.17Ga0.83N epilayer grown on a-plane (1 1 -2 0) GaN / (1 -1 0 2) r-plane sapphire substrate. The structure hence grown when investigated for photo-detecting properties, showed sensitivity to both infrared and ultraviolet radiations due to the different composition of InGaN region. Chapter 8 concludes with the summary of present investigations and the scope for future work.

Die vorliegende Arbeit beschaeftigt sich mit dem strukturellen Aufbau von (1-100) M-plane GaN, das mit plasmaunterstuetzter Molekularstrahlepitaxie auf gamma-LiAlO2(100) Substraten gewachsen wurde. Die heteroepitaktische Ausrichtung einerseits, sowie die Mikrostruktur und die Erzeugungsmechanismen der Defekte andererseits, wurde mit der Transmissionselektronenemikroskopie (TEM) systematisch untersucht. Das gamma-LiAlO2 Substrat reagiert heftig im Mikroskop unter Bestrahlung mit hochenergetischen Elektronen. Waehrend dieser Strahlenschaedigung verliert das Material seine urspruengliche kristalline Struktur und vollzieht eine Phasentransformation, die anhand einer Serie von Feinbereichsbeugungsdiagrammen nachgewiesen werden konnte. Die atomare Grenzflaechenstruktur zwischen epitaktisch gewachsenem alpha-GaN(1-100) und tetragonalem gamma-LiAlO2 Substrat ist mittels HRTEM untersucht worden. Die neuartige Epitaxiebeziehung ist mit Elektronenbeugung bestaetigt worden und lautet folgendermassen: (1-100)GaN liegt parallel zu (100)gamma-LiAlO2 und [11-20]GaN ist parallel zu [001]gamma-LiAlO2. Die Realstruktur der M-plane GaN Schichten, die auf (100)gamma-LiAlO2 gewachsen werden, unterscheidet sich erheblich von der in C-plane Orientierung hergestellten Epischichten. Ausfuehrliche TEM Untersuchungen zeigen, dass die M-plane Schichten vor allem intrinsische (I1 und I2) und extrinsische (E) Stapelfehler in der Basalebene enthalten. Der vorherrschende I2 Stapelfehler besitzt keine Komponente des Verschiebungsvektors senkrecht zur Ebene und ist damit nicht geeignet, epitaktische Dehnung entlang der [11-20] Richtung abzubauen. Darueberhinaus ist eine komplexe Grenze in der (10-10) Prismen- flaeche entdeckt worden, die zur Grenzflaeche geneigt verlaeuft. Die Defekte in den M-plane GaN Epischichten werden waehrend der anfaenglichen Keimbildungsphase erzeugt. Atomare Stufen entlang der [001] Richtung auf dem LiAlO2 Substrat fuehren zur Bildung von Stapelfehlern vom Typ I2. / In this work the structure of (1-100)M-plane GaN epitaxially grown on gamma-LiAlO2(100) by using plasmaassisted molecular beam epitaxy (PAMBE) is studied. The heteroepitaxial alignment and the microstructure of M-plane GaN as well as the defect formation in the layer are systematically investigated by using transmission electron microscopy (TEM). The gamma-LiALO2 substrate reacts under irradiation of high-energy electrons in the TEM (200-300 keV).The material looses its original crystalline structure during this process undergoing irradiation damage followed by a phase transformation as it is verified by a series of selected area diffraction patterns taken under constant electron dose. The result is a structural phase transformation from the tetragonal gamma to the trigonal alpha phase. The atomic interface structure of epitaxially grown hexagonal alpha-GaN(1-100) layers on tetragonal gamma-LiAlO2 (100) substrates is investigated by means of HRTEM. The novel epitaxial orientation relationship verified by electron diffraction is given by (1-100)GaN parallel to (100)gamma-LiAlO2 and [11-20]GaN parallel to [001]gamma-LiAlO2. The defect structure of M-plane GaN epilayers grown on gamma-LiAlO2(100) substrates is different to that of C-plane GaN. Our detailed TEM studies reveal that the M-plane layers mainly contain intrinsic I1 and I2 and extrinsic E basal plane stacking faults. The dominant I2 stacking fault has no out-of-plane displacement vector component and is thus not qualified for epitaxial strain relief along the [11-20] axis. Beyond this, a complex type of planar defect is detected in the (10-10) prism plane which is inclined with respect to the interface. The study of nucleation samples shows that the surface morphology is directly correlated to the generation of the dominant planar defects. Atomic steps along the [001] direction in the gamma-LiAlO2 substrate result in the formation of basal plane stacking faults I2.

Group III-A nitrides (GaN, AlN, InN and alloys) are materials of considerable contemporary interest and currently enable a wide variety of optoelectronic and high-power, high-frequency electronic applications. All of these applications utilize device structures that employ a single or multiple hetero-junctions, with material compositions varying across the interface. For example, the workhorse of GaN based electronic devices is the high electron mobility transistor (HEMT) which is usually composed of an AlGaN/GaN hetero-junction, where a two-dimensional electron gas (2DEG) is formed due to differences in polarization between the two layers. In addition to such hetero-junctions in the same material family, formation of hetero-interfaces in nitrides begins right from the epitaxy of the very first layer due to the lack of native substrates for their growth. The consequences of such "dissimilar" hetero-junctions typically manifest as large defect densities at this interface which in turn gives rise to defective films. Additionally, if the substrate is also a semiconductor, the electrical properties at such dissimilar semiconductor-nitride hetero-junctions are particularly important in terms of their influence on the performance of nitride devices. Nevertheless, the large defect densities at such dissimilar 3D-3D semiconductor interfaces, which translate into more trap states, also prevents them from being used as active device layers to say nothing of reliability considerations arising because of these defects. Recently, the advent of 2D materials such as graphene and MoS2 has opened up avenues for Van der Waal’s epitaxy of these layered films with practically any other material. Such defect-free integration enables dissimilar semiconductor hetero-junctions to be used as active device layers with carrier transport across the 2D-3D hetero-interface. This thesis deals with hetero-epitaxial growth platforms for reducing defect densities, and the material and electrical properties of dissimilar hetero-junctions with the group III-A nitride material system.