In this thesis the layered, two-dimensional material MoTe2 is examined experimentally for its optoelectronic properties, using a field effect transistor device configuration. MoTe2 experiences a strong light matter interaction, which is highly dependent on the conditions of the measurement, and the wavelength of light used. Light is able to: produce a photocurrent in MoTe2, desorb adsorbates from the surface, and even controllably thin by a single layer at a time. A theoretical study on MoTe2 also provides insights on the source of some of these interesting light matter interactions. MoTe2 is found to be a fast and responsive photodetector when illuminated with red laser light in ambient conditions, with increases in current stemming from the photovoltaic effect. Due to the generated charge carriers from the photovoltaic effect, conductivity can increase by increasing the Fermi energy of the material, or by a photogating effect where excited charges are trapped and behave as an artificial gate for the field effect transistor. The mechanisms of charge trapping are experimentally investigated due to their prevalence in the photodetection mechanisms. A theoretical study points towards the existence of two types of trap states, in not just MoTe2 but all transition metal dichalcogenides, with shallow traps closer to the valence band edge (τ ~ 500 s) and deeper traps (τ ~ 1000 s), further away from the valence band edge. MoTe2, under the effects of higher energy photons from blue and green lasers, showed different photocurrent mechanisms to red light. From the increased energy of the photons, photo-desorption of adsorbates on the surface of MoTe2 occurred causing a decrease in the overall current, in a rarely seen photocurrent mechanism. Again, both shallow and deep traps are evident from the experimental measurements, with the shallow traps being removed when illuminated by higher energy photons. Finally, a humidity assisted photochemical layer-by-layer etching process was developed with an in-situ Raman spectroscopy system, able to thin MoTe2 by a single layer at a time with 200 nm spatial resolution. MoTe2 FETs were created with thinned channels to examine the effect of the thinning technique on optoelectronic properties. Some improvement in optoelectronic performance (higher responsivity, higher mobility) was seen for the thinned channel devices, with great improvement observed for monolayer MoTe2.

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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.