Molecular Beam Epitaxy Growth of Transition Metal Dichalcogenides
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The exponential growth of Si-based technology has finally reached its limit, and a new generation of devices must be developed to continue scaling. A unique class of materials, transition metal dichalcogenides (TMD), have attracted great attention due to their remarkable optical and electronic properties at the atomic thickness scale. Over the past decade, enormous efforts have been put into TMD research for application in low-power devices. Among these studies, a high-quality TMD synthesis method is essential. Molecular beam epitaxy (MBE) can enable high-quality TMD growth by combining high purity elemental sources and an ultra-high vacuum growth environment, together with the back-end-of-line compatible growth temperatures. Although many TMD candidates have been grown by MBE with promising microstructure, the limited grain size (< 200 nm) for the MBE-grown TMDs reported in the literature thus far is unsuitable for high-performance device applications. In this dissertation, the synthesis of TMDs by MBE and their implementation in device structures were investigated. van der Waals epitaxial growth of these TMDs (HfSe2, WTe2, WSe2, WTexSe2-x), due to the relaxed interactions at the interface, have been demonstrated on large lattice-mismatched substrates without strain and misfit dislocations. The fundamental nucleation and growth behavior of WSe2 was investigated through a detailed experimental design, combined with on-lattice, diffusion-based first principles kinetic modeling. Over one order of magnitude improvement in grain size was achieved through this study. Results from both experiment and simulation showed that reducing the growth rate, enabled by high growth temperature and low metal flux, is vital to nucleation density control. Meanwhile, providing a chalcogen-rich growth environment will promote larger grain lateral growth by suppressing vertical growth. Applying the knowledge learned from the nucleation study, we sucessfully integrated the MBE-grown WSe2 into Si complementary metal-oxide-semiconductor (CMOS) compatible field-effect transistors (FETs). Excellent transport properties, such as field effect hole mobilities (40 cm2/V∙s) with orders of magnitude improvement over the reported values of MBE-grown TMDs, are shown. These studies provide a comprehensive understanding of the MBE synthesis of TMDs and devices, indicating the great potential of integrating TMDs into CMOS process flows for the future electronics.