Two-dimensional (2D) materials show novel electronic, optical and chemical properties and have great potential in devices such as field-effect transistors (FET), photodetectors and gas sensors. This thesis focuses on scanning tunneling microscopy and spectroscopy (STM/STS) investigation of interfaces and defects 2D transition metal dichalcogenides (TMDCs).
The first part of the thesis focuses on the synthesis of 2D TiSe2 with chemical vapor transport (CVT). By properly choosing the growth condition, Sub-10 nm TiSe2 flakes were successfully obtained. A 2 × 2 charge density wave (CDW) was clearly observed on these ultrathin flakes by scanning tunneling microscopy (STM). Accurate CDW phase transition temperature was measured by transport measurements. This work opens up a new approach to synthesize TMDCs.
The second part of the thesis focuses on monolayer vacancy islands growing on TiSe2 surface under electrical stressing. We have observed nonlinear area evolution and growth from triangular to hexagonal driven by STM subjected electrical stressing. Our simulations of monolayer island evolution using phase-field modeling and first-principles calculations are in good agreement with our experimental observations. The results could be potentially important for device reliability in systems containing ultrathin TMDCs and related 2D materials subject to electrical stressing.
The third part of the thesis focuses on point defects in 2D PtSe2. We observed five types of distinct defects from STM topography images and measured the local density of states (LDOS) of those defects from scanning tunneling spectroscopy (STS). We identified the types and characteristics of these defects with the first-principles calculations. Our findings would provide critical insight into tuning of carrier mobility, charge carrier relaxation, and electron-hole recombination rates by defect engineering or varying growth condition in few-layer 1T-PtSe2 and other related 2D materials. / Doctor of Philosophy / Since the discovery of graphene in 2004, two-dimensional (2D) materials have attracted more and more attentions. When the thickness of a layered material thinned to one or few atoms, it shows interesting properties different from its bulk phase. Due to the reduced dimensionality, interfaces and defects in 2D materials will significantly affect the electronic property and chemical activity. However, such nanometer scale features are several orders of magnitude smaller than the wavelength of visible light, which is the limit of resolution for optical microscope. Scanning tunneling microscope (STM) is widely used in study of 2D materials not only because it can provide the topography and local electronic information at atomic scale, but also because of the possibility of directly fabricate atomic scale structure on the surface.
The first part of the thesis focuses on the synthesis of 2D TiSe2 with chemical vapor transport (CVT). TiSe2 belongs to the transition metal dichalcogenides (TMDCs) family, showing a sandwiched layered structure. When the temperature goes down to 200K, a 2 × 2 superlattice called charge density wave (CDW) will show up, which is clearly observed in our STM images.
The second part of the thesis focuses on monolayer vacancy islands growing on TiSe2 surface controlled by electrical stressing. During continuous STM scanning, we have observed nonlinear area growth of the vacancy islands. The shape of those islands transfers from triangular to hexagonal. We successfully simulated such growth using phase-field modeling and first-principles calculations. The results could be potentially important for device reliability in systems containing ultrathin TMDCs and related 2D materials subject to electrical stressing.
The third part of the thesis focuses on defects in 2D PtSe2. We observed five types of distinct defects in our STM topography images. By comparing them with DFT-calculated simulation images, we identified the types and characteristics of these defects. Our findings would provide critical insight into tuning of carrier mobility, charge carrier relaxation, and electron-hole recombination rates by defect engineering in few-layer 1T-PtSe2 and other related 2D materials.
| Identifer | oai:union.ndltd.org:VTETD/oai:vtechworks.lib.vt.edu:10919/97440 |
| Date | 23 March 2020 |
| Creators | Zheng, Husong |
| Contributors | Physics, Tao, Chenggang, Robinson, Hans D., Heflin, James R., Park, Kyungwha |
| Publisher | Virginia Tech |
| Source Sets | Virginia Tech Theses and Dissertation |
| Detected Language | English |
| Type | Dissertation |
| Format | ETD, application/pdf, application/pdf, application/pdf, application/pdf, application/pdf, application/pdf, application/pdf |
| Rights | In Copyright, http://rightsstatements.org/vocab/InC/1.0/ |
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