On Demand Nanoscale Phase Manipulation of Vanadium Dioxide by Scanning Probe Lithography

This dissertation focuses on nanoscale phase manipulations of Vanadium Dioxide. Nanoscale control of material properties is a current obstacle for the next generation of optoelectronic and photonic devices. Vanadium Dioxide is a strongly correlated material with an insulator-metal phase transition at approximately 345 K that generates dramatic electronic and optical property changes. However, the development of industry device application based on this phenomenon has been limited thus far due to the macroscopic scale and the volatile nature of the phase transition. In this work these limitations are assessed and circumvented. A home-built, variable temperature, scanning near-field optical microscope was engineered for Vanadium Dioxide manipulations and detections. Using this instrument, various scanning probe lithography based methods are implemented to induce new nanoscale phases. Three new phase transitions are discovered; a monoclinic metallic at the nanoscale, a rutile metallic metastable phase, and a van der Waals layered insulator. These new phases are studied and characterized to further understand phase manipulations in strongly correlated materials. One of the new phase transitions, monoclinic metallic, showcases plasmonic excitations. This phenomenon is used to demonstrate various nanoplasmonic devices such as rewritable waveguides, spatially modulated resonators, and reconfigurable planar optics. Finally, Oxygen Vacancy diffusion of the monoclinic structure is monitored to determine the temporal limitation for device applications. The discovery, demonstration, and study of these phases clearly shows the ability to manipulate Vanadium Dioxide on the nanoscale for the first time. Phase control is accomplished under ambient conditions and is stable over long periods of time. This technology opens the door for multifunctional device application using strongly correlated materials

Design of Scattering Scanning Near-Field Optical Microscope

The primary objective of this work is to construct a fully functional scattering type Scanning Near-field Optical Microscope (s-SNOM), and to understand the working mechanisms behind it. An s-SNOM is an instrument made up of two separate instruments working in unison. One instrument is a scanning optical microscope focusing light onto a raster scanning sample surface combined with an interferometer set up. The second instrument is an Atomic Force Microscope (AFM) operating in noncontact mode. The AFM uses a small probe that interacts with the raster scanning sample surface to map out the topography of the of the sample surface. An s-SNOM uses both of these instruments simultaneously by focusing the light of the optical microscope onto the probe of the AFM. This probe acts as a nano-antenna and confines the light allowing for light-matter interaction to be inferred far below the resolution of the diffraction limit of light. This specific s-SNOM system is unique to others by having a controllable environment. It is high vacuum compatible and variable temperature. In addition, it is efficient at collecting scattered light due to the focusing objective being a partial elliptical mirror which collects 360° of light around the major axis. This s-SNOM system will be used for direct imaging of surface plasmons. Intended works are inducing surface plasmons on InSe thin films, and seeing the enhancement effect of introducing Au nano-rods. Also dielectric properties of materials will be interpreted such as the metal to insulator phase transition of NbO2

Multiferroic BaCoF4 in Thin Film Form: Ferroelectricity, Magnetic Ordering, and Strain.

Multiferroic materials have simultaneous magnetic and ferroelectric long-range orders and can be potentially useful for a wide range of applications. Conventional ferroelectricity in oxide perovskites favors nonmagnetic electronic configurations of transition metal ions, thus limiting the number of intrinsic multiferroic materials. On the other hand, this is not necessarily true for multiferroic fluorides. Using molecular beam epitaxy, we demonstrate for the first time that the multiferroic orthorhombic fluoride BaCoF4 can be synthesized in thin film form. Ferroelectric hysteresis measurements and piezoresponse force microscopy show that the films are indeed ferroelectric. From structural information, magnetic measurements, and first-principles calculations, a modified magnetic ground state is identified which can be represented as a combination of bulk collinear antiferromagnetism with two additional canted spin orders oriented along orthogonal axes of the BaCoF4 unit cell. The calculations indicate that an anisotropic epitaxial strain is responsible for this unusual magnetic ground state

Multiferroic BaCoF4 in Thin Film Form: Ferroelectricity, Magnetic Ordering, and Strain.

Multiferroic materials have simultaneous magnetic and ferroelectric long-range orders and can be potentially useful for a wide range of applications. Conventional ferroelectricity in oxide perovskites favors nonmagnetic electronic configurations of transition metal ions, thus limiting the number of intrinsic multiferroic materials. On the other hand, this is not necessarily true for multiferroic fluorides. Using molecular beam epitaxy, we demonstrate for the first time that the multiferroic orthorhombic fluoride BaCoF4 can be synthesized in thin film form. Ferroelectric hysteresis measurements and piezoresponse force microscopy show that the films are indeed ferroelectric. From structural information, magnetic measurements, and first-principles calculations, a modified magnetic ground state is identified which can be represented as a combination of bulk collinear antiferromagnetism with two additional canted spin orders oriented along orthogonal axes of the BaCoF4 unit cell. The calculations indicate that an anisotropic epitaxial strain is responsible for this unusual magnetic ground state