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.

This thesis describes the fabrication and characterization of two-dimensional transition dichalcogenides (2D TMDs) nanolayers for various applications in electronic and opto-electronic devices applications. In Chapter 1, crystal and optical structure of TMDs materials are introduced. Many TMDs materials reveal three structure polytypes (1T, 2H, and 3R). The important electronic properties are determined by the crystal structure of TMDs; thus, the information of crystal structure is explained. In addition, the detailed information of photon vibration and optical band gap structure from single-layer to bulk TMDs materials are introduced in this chapter. In Chapter 2, detailed information of physical properties and synthesis techniques for molybdenum disulfide (MoS2), tungsten disulfide (WS2), and molybdenum ditelluride (MoTe2) nanolayers are explained. The three representative crystal structures are trigonal prismatic (hexagonal, H), octahedral (tetragonal, T), and distorted structure (Tʹ). At room temperature, the stable structure of MoS2 and WS2 is semiconducting 2H phase, and MoTe2 can reveal both 2H (semiconducting phase) and 1Tʹ (semi-metallic phase) phases determined by the existence of strains. In addition, the pros and cons of the synthesis techniques for nanolayers are discussed. In Chapter 3, the topic of synthesized large-scale MoS2, WS2, and MoTe2 films is considered. For MoS2 and WS2 films, the layer thickness is modulated from single-layer to multi-layers. The few-layer MoTe2 film is synthesized with two different phases (2H or 1Tʹ). The all TMDs films are fabricated using two-step chemical vapor deposition (CVD) method. The analyses of atomic force microscopy (AFM), high-resolution transmission electron microscopy (HRTEM), photoluminescence (PL), and Raman spectroscopy confirm that the synthesis of high crystalline MoS2, WS2, and MoTe2 films are successful. The electronic properties of both MoS2 and WS2 exhibit a p-type conduction with relatively high field effect mobility and current on/off ratio. In Chapter 4, vertically-stacked few-layer MoS2/WS2 heterostructures on SiO2/Si and flexible polyethylene terephthalate (PET) substrates is presented. Detailed structural characterizations by Raman spectroscopy and high-resolution/scanning transmission electron microscopy (HRTEM/STEM) show the structural integrity of two distinct 2D TMD layers with atomically sharp van der Waals (vdW) heterointerfaces. Electrical transport measurements of the MoS2/WS2 heterostructure reveal diode-like behavior with current on/off ratio of ~ 104. In Chapter 5, optically uniform and scalable single-layer Mo1-xWxS2 alloys are synthesized by a two-step CVD method followed by a laser thinning. Post laser treatment is presented for etching of few-layer Mo1-xWxS2 alloys down to single-layer alloys. The optical band gap is controlled from 1.871 to 1.971 eV with the variation in the tungsten (W) content, x = 0 to 1. PL and Raman mapping analyses confirm that the laser-thinning of the Mo1-xWxS2 alloys is a self-limiting process caused via heat dissipation to SiO2/Si substrate, resulting in fabrication of spatially uniform single-layer Mo1-xWxS2 alloy films.