Browsing by Author "Khodaparast, Giti"
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- Computational Design of 2D-Mechanical MetamaterialsMcMillan, Kiara Lia (Virginia Tech, 2022-06-22)Mechanical metamaterials are novel materials that display unique properties from their underlying microstructure topology rather than the constituent material they are made from. Their effective properties displayed at macroscale depend on the design of their microstructural topology. In this work, two classes of mechanical metamaterials are studied within the 2D-space. The first class is made of trusses, referred to as truss-based mechanical metamaterials. These materials are studied through their application to a beam component, where finite element analysis is performed to determine how truss-based microstructures affect the displacement behavior of the beam. This analysis is further subsidized with the development of a graphical user interface, where users can design a beam made of truss-based microstructures to see how their design affects the beam's behavior. The second class of mechanical metamaterial investigated is made of self-assembled structures, called spinodoids. Their smooth topology makes them less prone to high stress concentrations present in truss-based mechanical metamaterials. A large database of spinodoids is generated in this study. Through data-driven modeling the geometry of the spinodoids is coupled with their Young's modulus value to approach inverse design under uncertainty. To see mechanical metamaterials applied to industry they need to be better understood and thoroughly characterized. Furthermore, more tools that specifically help push the ease in the design of these metamaterials are needed. This work aims to improve the understanding of mechanical metamaterials and develop efficient computational design strategies catered solely for them.
- Decoherence of Transverse Electronic Spin Current in Magnetic MetalsLim, Youngmin (Virginia Tech, 2022-05-31)Transport of spin angular momentum (spin currents) in magnetic thin films is important for non-volatile spin-based memory devices and other emerging information technology applications. It is especially important to understand how a spin current propagates across interfaces and how a spin current interacts with magnetic moments. The great interest in devices based on ferromagnetic metals generated intensive theoretical and experimental studies on the basic physics of spin currents for the last few decades. Of particular interest recently is the so-called "pure" electronic spin current, which is carried by electrons and yet unaccompanied by net charge flow, in part because of the prospect of transporting spin with minimal Joule heating. However, in contrast to ferromagnetic metals, spin transport in antiferromagnetic metals, which are promising materials for next-generation magnetic information technology, is not well understood yet. This dissertation addresses the mechanisms of transport by pure spin current in thin-film multilayers incorporating metals with antiferromagnetic order. We focus on two specific materials: (1) CoGd alloys with ferrimagnetic sublattices, which resemble antiferromagnets near the compensation composition, and (2) elemental antiferromagnetic Cr, which can be grown as epitaxial films and hence serve as a model system material. For both the CoGd and Cr studies, spin-valve-like structures of NiFe/Cu/CoGd and NiFe/Cu/Cr/CoFe are prepared to conduct ferromagnetic resonance spin pumping experiments. Precessing magnetization in the NiFe "spin source" pumps a transverse spin current to the adjacent layers. We measure the loss of the spin angular momentum in the "spin sink" layer by measuring the broadening of the resonance linewidth, i.e., the non-local damping enhancement, of the spin source. The antiparallel magnetic moments of Co and Gd sublattices partially cancel out the dephasing of a transverse spin current, thereby resulting in a long spin dephasing length of ≈ 5-6 nm near the magnetic compensation point. We find evidence that the spin current interacts somewhat more strongly with the itinerant transition-metal Co magnetism than the localized rare-earth-metal Gd magnetism in the CoGd alloy. We also examine spin transport via structurally clean antiferromagnetic Cr, epitaxially grown with BCC crystal order. We observe strong spin reflection at the Cu/Cr interface, which is surprising considering that thin layers of Cu and Cr individually are transparent to spin currents carried by electrons. Further, our results indicate other combinations of electrically conductive elemental metals (e.g., Cu/V) can form effective spin-reflecting interfaces. Overall, this thesis advances the basic understanding of spin transport in metallic thin films with and without magnetic order, which can aid the development of next generations of efficient spintronic devices. This work was supported in part by the National Science Foundation, Grant No. DMR-2003914.
- Epitaxial Gallium Oxide Heterojunctions for Vertical Power RectifiersSpencer, Joseph Andrew (Virginia Tech, 2024-06-03)At the heart of all power electronic systems lies the semiconductor, responsible for passing large amounts of current at negligible power losses in the on-state, while instantaneously switching to withstand high voltages in the off-state. For decades silicon (Si) has dominated nearly all aspects of electronic systems including power. As importunity for efficiency at higher power and fast switching speeds grows, the environments with which these systems are being tasked to operate in has also increased in rigor. This has placed semiconductors at the forefront of innovation as novel materials are being explored in hopes of meeting the demands for the future of power electronics. This exploration of novel materials for power electronics has come to fruition as the performance limits of narrow bandgap (EG) materials such as Si (1.1 eV) have been reached. The EG is a key measure of a materials ability to operate at high voltages and within high temperature environments. This is due to the direct relationship of the EG to the critical field strength which enables increased performance beyond that of narrow band gap materials such as Si and gallium arsenide. Wide bandgap (WBG) materials such as silicon carbide (SiC) and gallium nitride (GaN) with EG 3.3 eV and 3.4 eV, respectively, have emerged within the power electronics field to offer increased breakdown voltages (VBR) at lower on-resistances. However, ultrawide bandgap (UWBG) devices possess greater potential with superior performance limits in comparison to SiC and GaN. Ga2O3 (4.8 eV) is the only UWBG semiconductor with melt-growth capabilities that has already demonstrated research grade wafers up to 6" in diameter. Ga2O3 is also advantaged by the ability to grow thick, lowly-doped homoepitaxial drift regions from methods such as halide vapor phase epitaxy (HVPE) and metal organic chemical vapor deposition (MOCVD). This makes Ga2O3 a prime candidate for vertical power rectifiers as thick, high quality drift regions are a necessity for high voltage devices such as the PN diode, junction barrier Schottky (JBS) diode, merged-PiN-Schottky (MPS) diode, and Schottky barrier diode (SBD). However, Ga2O3 exhibits a lack of p-type conductive that arises from an absence of dispersion within the valence band maximum. This has caused researchers to abandon the idea of homojunction devices that Si, SiC, and GaN devices benefit from; shifting to a heterojunction approach where NiO (3.7 eV) provides the source of p-type conductivity. This complicates fabrication and device characterization particularly for the Ga2O3 JBS diode where an etched Ga2O3-NiO heterojunction has thus far been unreported throughout the literature. This work investigates the numerous individual aspects that comprise an etched Ga2O3 heterojunction device which include the etching method, post etch damage removal and its impact on electrical performance, and ohmic and Schottky contacts critical for a JBS diode; all culminating in the demonstration of a JBS and MPS diodes. We also report our investigations into co-doping of Ga2O3 that yield degenerately doped epitaxial layers with record mobility (μ) values. While not directly correlated with Ga2O3-NiO heterojunction devices, this study lays the ground work for semi-insulating Ga2O3 depletion into unintentionally doped (UID) n-type Ga2O3.
- Gamma-ray emission from Galactic millisecond pulsars: Implications for dark matter indirect detectionSong, Deheng (Virginia Tech, 2022-01-18)The Fermi Large Area Telescope has observed a gamma-ray excess toward the center of the Galaxy at ~ GeV energies. The spectrum and intensity of the excess are consistent with the annihilation of dark matter with a mass of ~100 GeV and a velocity-averaged cross section of ~ 1e-26 cubic centimeter per second. In the meantime, a population of unresolved millisecond pulsars (MSPs) in the Galactic center remains a possible source of the excess. Furthermore, recent analyses have shown that the excess prefers the spatial morphology of the stellar bulge distribution in the Galactic center, supporting a MSP origin. The new discovery makes it imperative to further study the signals from MSPs. This dissertation studies the gamma-ray emission from Galactic millisecond pulsars to provide new insights into the origin of the Galactic center excess. Using the GALPROP code, we simulate the propagation of e± injected by the putative MSPs in the Galactic bulge and calculate the inverse Compton (IC) emission caused by the e± losing energy in the interstellar radiation field. We find recognizable features in the spatial maps of the IC. Above TeV energies, the IC morphology tends to follow the distribution of the injected e±. Then, we study the Cherenkov Telescope Array (CTA) sensitivity to the IC signal from MSPs. We find that the CTA has the potential to robustly discover the IC signature when the MSP e± injection efficiencies are in the range ≈ 2.9-74.1%. The CTA can also discriminate between an MSP and a dark matter origin for the radiating e± based on their different spatial maps. Next, we analyze the Fermi data from directions of Galactic globular clusters. The globular clusters are thought to be shining in gamma rays because of the MSP population they host. By analyzing their gamma-ray spectra, we reveal evidence for an IC component in the high-energy tail of Fermi data. Based on the IC component in the globular cluster spectra, the e± injection efficiency of millisecond pulsars is estimated to be slightly smaller than 10%. Finally, we study the spatial morphology of the 511 keV signal toward the Galactic center using data from INTEGRAL/SPI. We confirm that the 511 keV signal also traces the old stellar population in the Galactic bulge, which is similar to the Fermi GeV excess. Using a 3D smoothing kernel, we find that the signal is smeared out over a characteristic length scale of 150 ± 50 pc. We show that positron propagation prior to annihilation can explain the overall phenomenology of the 511 keV signal.
- Half-Heusler Thermoelectric Materials and ModulesKang, Han-Byul (Virginia Tech, 2019-08-29)High temperature waste heat recovery has been gaining attention in recent years as it forms one of the largest sources of available energy. A rapid development of thermoelectric (TE) materials that can directly convert heat into electricity through the Seebeck effect, opens promising pathway for harvesting the thermal energy from the surroundings. In order to harvest the high-quality waste heat at elevated temperature, excellent thermal and mechanical stability of the TE materials is critical for a sustainable energy harvesting. In this respect, half-Heusler (hH) alloys are one of the promising high-temperature TE materials due to their high dimensionless thermoelectric figure of merit (zT) along with excellent mechanical and thermal stability. This dissertation demonstrates novel hH compositions and microstructures for the waste heat recovery systems. Focus in the thesis is on development of high performance hH TE materials with excellent in-air thermal stability at high temperatures (>700K). This will allow manufacturing of high efficiency and durable high temperature thermoelectric generators (TEGs). In chapter 3 and 4, a comprehensive optimization of n-type MNiSn and p-type MCoSb (M = Hf, Zr, and Ti) compounds is investigated through systematic control of processing parameters during melting and sintering. The synthesis conditions were controlled to achieve the phase purity, desired microstructure and the enhanced charge-carrier transport. Optimized n-type and p-type compositions are found to exhibit zTmax ~ 1 at 773 K. Chapter 5 describes breakthrough in decoupling of TE parameters in n-type half-Heusler (hH) alloys through multi-scale nanocomposite architecture with tungsten nanoinclusions. The tungsten nanoparticles not only assist electron injection, thereby improving electrical conductivity, but also enhance the Seebeck coefficient through energy filtering effect. The microstructure comprises of disordered phases with feature sizes at multiple length scales, which assists in effective scattering of heat-carrying phonons over diverse mean-free-path ranges. Cumulatively, these effects are shown to result in outstanding thermoelectric performance of zTmax ~ 1.4 at 773 K and zTavg ~ 0.93 between 300 and 973 K. In order to deploy TE materials into a thermal energy conversion device, it is essential to understand the transformation behavior under thermal cycling at high temperatures. In-air thermal stability of the hH compositions is demonstrated in chapter 6. All the optimized compositions are found to be stable below 673 K in-air condition. The n-type MNiSn and p-type NbFeSb compounds were found to show good thermal stability even at higher temperatures (>773K), whereas MCoSb compounds did not exhibit similar level of stability. Building upon the improved material performance and thermal stability, uni-coupled TE generators are demonstrated that exhibit high power density of 13.81 W⸱cm-2 and conversion efficiency of 10.9 % under a temperature difference of 674 K. The uni-couple TEG device shows stable performance for more than 150 hours at 873 K in air. These results are very promising for deployment of TE materials in waste heat recovery systems.
- Multiresonant Plasmonics with Spatial Mode OverlapSafiabadi Tali, Seied Ali (Virginia Tech, 2022-02-03)Plasmonic nanostructures can enhance light-matter interactions in the subwavelength domain, which is useful for photodetection, light emission, optical biosensing, and spectroscopy. However, conventional plasmonic devices are optimized to operate in a single wavelength band, which is not efficient for wavelength-multiplexed operations and quantum optical applications involving multi-photon nonlinear processes at multiple wavelength bands. Overcoming the limitations of single-resonant plasmonics requires development of plasmonic devices that can enhance the optical interactions at the same locations but at different resonance wavelengths. This dissertation comprehensively studies the theory, design, and applications of such devices, called "multiresonant plasmonic systems with spatial mode overlap". We start by a literature review to elucidate the importance of this topic as well as its current and potential applications. Then, we briefly discuss the fundamentals of plasmonic resonances and mode hybridization to thoroughly explore, classify, and compare the different architectures of the multiresonant plasmonic systems with spatial mode overlap. Also, we establish the black-box coupled mode theory to quantify the coupling of optical modes and analyze the complicated dynamics of optical interactions in multiresonant plasmonic systems. Next, we introduce the nanolaminate plasmonic crystals (NPCs), wafer-scale metamaterials structures that support many (>10) highly-excitable plasmonic modes with spatial overlap across the visible and near-infrared optical bands. The enabling factors behind the NPC's superior performance as multiresonant systems are also theoretically and experimentally investigated. After that, we experimentally demonstrate the NPCs application in simultaneous second harmonic generation and anti-Stokes photoluminescence (ASPL) with controllable nonlinear emission properties. By designing specific non-linear optical experiments and developing advanced ASPL models, this work addresses some important but previously unresolved questions on the ASPL mechanism as well. Finally, we conclude the dissertation by discussing the potential applications of out-of-plane plasmonic systems with spatial mode overlap in wavelength-multiplexed devices and presenting some preliminary results.
- Multivalley Electron Conduction at the Indirect-Direct Crossover Point in Highly Tensile-Strained GermaniumClavel, Michael B.; Murphy-Armando, F.; Xie, Y.; Henry, K.; Kuhn, M.; Bodnar, Robert J.; Khodaparast, Giti; Smirnov, D.; Heremans, Jean; Hudait, Mantu K. (American Physical Society, 2022-12-01)As forward-looking electron devices increasingly adopt high-mobility low-band-gap materials, such as germanium (Ge), questions remain regarding the feasibility of strain engineering in low-band-gap systems. Particularly, the Ge L-Γ valley separation (∼150 meV) can be overcome by introducing a high degree of tensile strain (ε ≥ 1.5%). It is therefore essential to understand the nature of highly strained Ge transport, wherein multivalley electron conduction becomes a possibility. Here, we report on the competitiveness between L- and Γ-valley transport in highly tensile-strained (ε ∼ 1.6%) Ge/In0.24Ga0.76As heterostructures. Temperature-dependent magnetotransport analysis reveals two contributing carrier populations, identified as lower- and higher-mobility L- and Γ-valley electrons (in Ge), using temperature-dependent Boltzmann transport modeling. Coupling this interpretation with electron-cyclotron-resonance studies, the effective mass (m*) of the higher-mobility Γ-valley electrons is probed, revealing m* = (0.049 ± 0.007)me. Moreover, a comparison of empirical and theoretical m* indicates that these electrons reside primarily in the first-two quantum sublevels of the Ge Γ valley. Consequently, our results provide an insight into the strain-dependent carrier dynamics of Ge, offering alternative pathways toward efficacious strain engineering.
- Nanostructures for Coherent Light Sources and PhotodetectorsHo, Vinh Xuan (Virginia Tech, 2020-05-14)Large-scale optoelectronic integration is limited by the lack of efficient light sources and broadband photodetectors, which could be integrated with the silicon complementary metal-oxide-semiconductor (CMOS) technology. Persistent efforts continue to achieve efficient light emission as well as broadband photodetection from silicon in extending the silicon technology into fully integrated optoelectronic circuits. Recent breakthroughs, including the demonstration of high-speed optical modulators, photodetectors, and waveguides in silicon, have brought the concept of transition from electrical to optical interconnects closer to realization. The on-chip light sources based on silicon are still a key challenge due to the indirect bandgap of silicon that impedes coherent light sources. To overcome this issue, we have studied, fabricated, and characterized nanostructures including single semiconductor epilayers, multiple quantum wells, and graphene-semiconductor heterostructures to develop coherent light sources and photodetectors in silicon. To develop coherent light sources, we reported the demonstration of room-temperature lasing at the technologically crucial 1.5 m wavelength range from Er-doped GaN epilayers and Er-doped GaN multiple-quantum wells grown on silicon and sapphire. The realization of room-temperature lasing at the minimum loss window of optical fiber and in the eye-safe wavelength region of 1.5 m is highly sought-after for use in many applications in various fields including defense, industrial processing, communication, medicine, spectroscopy and imaging. The results laid the foundation for achieving hybrid GaN-Si lasers providing a new pathway towards full photonic integration for silicon optoelectronics. Silicon photodiodes contribute a large portion in the photodetector market. However, silicon photodetectors are sensitive in the UV to near infrared region. Photodetection in the mid-infrared is based on thermal radiation detectors, narrow bandgap materials (InGaAs, HgCdTe) semiconductors, photo-ionization of shallow impurities in semiconductors (Si:As, Ge:Ga), and quantum well structures. Such technology requires complicated fabrication processes or cryogenic operation, resulting in manufacturing costs and severe integration issues. To develop broadband photodetectors, we focus on graphene photodetectors on silicon. Graphene generates photocarriers by absorbing photons in a broadband spectrum from the deep-ultraviolet to the terahertz region. Graphene can be realized as the next generation broadband photodetection material, especially in the infrared to terahertz region. Here, we have demonstrated high-performance hybrid photodetectors operating from the deep-ultraviolet to the mid-infrared region with high sensitivity and ultrafast response by coupling graphene with a p-type semiconductor photosensitizer, nitrogen-doped Ta2O5 thin film.
- Novel Electrochemical Methods for Human NeurochemistryEltahir, Amnah (Virginia Tech, 2020-10-14)Computational psychiatry describes psychological phenomena as abnormalities in biological computations. Current available technologies span multiple organizational and temporal domains, but there remains a knowledge gap with respect to neuromodulator dynamics in humans. Recent efforts by members of the Montague Laboratory and collaborators adapted fast scan cyclic voltammetry (FSCV) from rodent experiments for use in human patients already receiving brain surgery. The process of modifying established FSCV methods for clinical application has led improved model building strategies, and a new "random burst" sensing protocol. The advent of random burst sensing raises questions about the capabilities of in-vivo electrochemistry techniques, while opening introducing possibilities for novel approaches. Through a series of in-vitro experiments, this study aims to explore and validate novel electrochemical sensing approaches. Initial expository experiments tested assumptions about waveform design to detect dopamine concentrations by reducing amplitude and duration of forcing functions, as well as distinguishing norepinephrine concentrations. Next, large data sets collected on mixtures of dopamine, serotonin and pH validated a newly proposed "low amplitude random burst sensing" protocol, for both within-probe and out-of-probe modeling. Data collected on the same set of solutions also attempted to establish an order-millisecond random burst sensing approach. Preliminary endeavors into using convolutional neural networks also provided an example of an alternative modeling strategy. The results of this work challenge existing assumptions of neurochemistry, while demonstrating the capabilities of new neurochemical sensing approaches. This study will also act as a springboard for emerging technological developments in human neurochemistry.
- Optical control and probe of ferromagnetic and ferroic orders in films, heterostructures, and perovskite-based material systemsSmith, Nicholas William (Virginia Tech, 2023-12-04)This dissertation is focused on ferromagnetic, multiferroics, and two-dimensional (2D) perovskites, exploring different unique collective magnetic and ferroic characters: (1) ferromagnetic thin film Co/Pd multilayers, (2) BaTiO3-BiFeO3 (BTO-BFO) a magneto-electric materials system, and (3) CuCl4 halide organic-inorganic perovskites. Low-power all-optical memory offers a unique opportunity to achieve ultra-fast magnetic switching in which the switching dynamics are not thermally mediated and occur on the order of the laser pulse. However, it is challenging to achieve a low-power optically excited magnetization precession angle above 90 degrees, which is required for magnetic switching. Co/Pd thin film multilayers were investigated for their potentially large perpendicular magnetic anisotropy (PMA) with three differing regimes of magnetic anisotropy: in-plane, weakly out-of-plane, and out-of-plane. Utilizing the time-resolved magneto-optical Kerr effect (TR-MOKE), we observed clear magnetic precession (on the order of a few GHz) with magnetic precession angle increasing (up to 4.5 degrees) for thinner Co samples which demonstrated stronger PMA. We observed a clear connection between PMA strength and precession amplitude as well as a large efficiency of energy transfer between spin and orbital subsystems for our strongest PMA sample. BTO-BFO is a strong room-temperature multiferroic with enhanced magneto-electric properties compared to BFO. We utilized time-resolved differential reflectivity (TR-DR) and TR-MOKE to observe strong coherent acoustic phonons in thin films as well as nanorods. Our nanorods showed additional modes (a new 20 GHz and 6 GHz mode) not observed in thin films including the fast 33 GHz mode which showed some weak tunability with high magnetic fields (up to 10 T). The observed tunability of these modes in an external magnetic field shows interesting coupling between magnetic moment and phononic modes which may be caused by the breaking of the spin-cycloid at the interface of the nanorods and the surface of the nanorods. We also observed second harmonic generation (SHG) emission which demonstrated a large enhancement in our nanorod structures with further observation of wavelength dependence. Finally, ferromagnetic resonance on our nanorod and thin film BTO-BFO structures indicated very weak Gilbert damping (on the order of 10−3), demonstrating the practicality of our structure for low-spin loss applications. Lastly, this dissertation focuses on a project around CuCl4 and CuCl2Br2 perovskites in which we observed time-dependent SHG. An increase in SHG as a function of infrared laser exposure is shown to coincide with changes in the crystal structure of the Cu perovskite materials. This increase in SHG was shown to last for a few days after hours of laser exposure indicating a slow hysteretic change to the crystal structure of the perovskites.
- Probing Coherent States and Nonlinear Properties in Multifunctional Material SystemsHerath Mudiyanselage, Rathsara Rasanjalee Herath (Virginia Tech, 2021-04-15)The rapid progress on developing new and improved multifunctional materials, for optoelectronic and spin based phenomena/devices, have increased the importance of the fundamental understanding of their coherent states and nonlinear optical properties. This study is aimed at characterizing, modeling, and controlling the fundamental electronic, phononic, and spin properties of several classes of materials through nonequilibrium and nonlinear light-matter interactions, coupled with a novel design of the material phases, interfaces, and heterostructures. This research directly addresses the Grand Challenges identified in the Basic Energy Sciences Advisory Committee report "Directing Matter and Energy: Five Challenges for Science and the Imagination" (Hemminger, 2007) [1], in particular, the area: "Matter far beyond equilibrium" and addresses the questions, "How do remarkable properties of matter emerge from complex correlations of the atomic or electronic constituents and how can we control these properties?" and "How do we design and perfect atom- and energy-efficient synthesis of revolutionary new forms of matter with tailored properties?". The knowledge gained from these fundamental studies can provide new information for a broad community to provide concepts for the next generation of multifunctional materials and devices, and resulted in several publications and conference presentations. The materials studied in this dissertation included multiferroic BaTiO3-BiFeO3 [2], ferroelectric Pb0.52Zr0.48TiO3 (PZT), InAs/AlAsSb multi-quantum-well [3], lead halide perovskite [4], n-type InAsP films [5, 6], and nanolaminate plasmonic crystals [7]. Probing multiferroics, which are materials that can exhibit ferromagnetic, ferroelectric, and ferroelastic orders simultaneously in a single phase, was a main focus of this study. BiFeO3 (BFO) is the most widely investigated multiferroic due to its high Neel and Curie temperatures and has antiferromagnetic and ferroelectric properties [8]. An inherent drawback of BFO is its large leakage currents. In this project, (1 − x)BaTiO3-(x)BiFeO3, x = 0.725 (BTO-BFO) heterostructures were investigated [9], where the conductivity of the solid solution can be reduced by adding another perovskite material, BaTiO3 [2]. We aimed to study optically induced coherent states in our BTO-BFO structures. Time resolved pumpprobe spectroscopic measurements were performed at room temperature as well as at low temperature (100 K) up to 10 T. Coherent acoustic phonons were observed both in a film and nanorods, resulting in coherent phonon frequencies of 27 and 33 GHz, respectively [2]. Coherent phonon spectroscopy is a sensitive tool to characterize the interfaces and can be employed as an effective ultrasensitive quantum sensor [10]. Furthermore, in the nanorods arrays of BTO-BFO, an additional oscillation with frequency in the range of 8.1 GHz was observed. This frequency is close to a theoretically predicted magnon frequency which could indicate the coexistence of coherent phonons and magnons in the nanorods arrays [2]. In an analogy to photonics which relies on electromagnetic waves, magnonics utilizes spin waves to carry and process information, offering several advantages such as an operation frequency in the THz range. Recently, "a quantum tango" [11] was reported where coupled coherent magnon and phonons modes were formed on a surface patterned ferromagnet. Furthermore, BTO-BFO heterostructures were probed using transient birefringence and magneto-optical Kerr effect spectroscopy. The results demonstrated that the magnetic field dependence of coherent phonons, measured by these two techniques, exhibits more sensitivity to the external magnetic fields compared to the differential reflectivity technique [2]. Moreover, nonlinear optical properties of this structure were investigated via second harmonic generation spectroscopy, where wavelength and polarization dependence of this nonlinear observation will be discussed in this dissertation. As part of this study, another class of multiferroic materials, with strong ferroelectric and piezoelectric properties, Pb0.52Zr0.48TiO3 (PZT) was studied [12]. In this project, the nonlinear optical properties of PZT nanorod arrays were investigated. Clear signatures of second harmonic generations from 490-525 nm (2.38-2.53 eV) at room temperature, were observed. Furthermore, time resolved differential reflectivity measurements were performed to study dynamical properties in the range of 690-1000 nm where multiphoton processes were responsible for the photoexcitations. We compared this excitation scheme, which is sensitive mainly to the surface states, to when the photoexcited energy (∼ 3.1 eV) was close to the bandgap of the nanorods. Our results offer promises for employing these nanostructures in nonlinear photonic applications. Furthermore, the established techniques during my research provided new insights on optical properties of InAs/AlAsSb multi-quantum-well [3], lead halide perovskite [4], n-type InAsP films [5, 6], and nanolaminate plasmonic crystals [7], and the results will be briefly presented in this dissertation.
- Probing Collective Motions and Hydration Dynamics of Biomolecules by a Wide Range Dielectric SpectroscopyCharkhesht, Ali (Virginia Tech, 2019-06-25)Studying dynamics of proteins in their biological milieu such as water is interesting because of their strong absorption in the terahertz range that contain information on their global and sub-global collective vibrational modes (conformational dynamics) and global dynamical correlations among solvent water molecules and proteins. In addition, water molecules dynamics within protein solvation layers play a major role in enzyme activity. However, due to the strong absorption of water in the gigahertz-to-terahertz frequencies, it is challenging to study the properties of the solvent dynamics as well as the conformational changes of protein in water. In response, we have developed a highly sensitive megahertz-to-terahertz dielectric spectroscopy system to probe the hydration shells as well as large-scale dynamics of these biomolecules. Thereby, we have deduced the conformation flexibility of proteins and compare the hydration dynamics around proteins to understand the effects of surface-mediated solvent dynamics, relationships among different measures of interfacial solvent dynamics, and protein-mediated solvent dynamics based on the complex dielectric response from 50 MHz up to 2 THz by using the system we developed. Comparing these assets of various proteins in different classes helps us shed light on the macromolecular dynamics in a biologically relevant water environment.
- Self-assembly of anisotropic nanostructures and interferometric spectroscopyHe, Zhixing (Virginia Tech, 2020-03-20)With the development of controlled and predictable nanoparticle fabrication, assembling multiple nano-objects into larger functional nanostructure has attracted increasing attention. As the most basic structure, assembly of one-dimensional (1D) structures is a good model for investigating the assembly mechanism of a nanostructure's formation from individual particles. In this dissertation, the dynamics and the growth mechanism of anisotropic 1D nanostructures is investigated. In our first study, we demonstrate a simple method for assembling superparamagnetic nanoparticles (SPIONs) into structure-controlled 1D chains in a rotating magnetic field. The length of the SPION chains can be well described by an exponential distribution, as is also seen in SPION chains in a static field. In addition, the maximum chain length is limited by the field's rotational speed, as is seen in micro-sized beads forming chains in a rotating field. However, due to a combination of thermal fluctuations and hydrodynamic forces, the chain length in our case is shorter than either limit. In addition to chain length, the disorder of chains was also studied. Because of the friction between particles, kinetic potential traps prevent relaxation to the global free energy minimum. The traps are too deep to be overcome through thermal fluctuations, and assemblies captured by the kinetic traps therefore form disordered chains. We demonstrate that this disorder gradually heals over a timescale of tens of minutes and that the healing process can be promoted by increasing particle concentration or solution ionic strength, suggesting that the chain growth process provides the energy required to overcome the kinetic trapping. Next, we introduce a novel optical technique we term Quantitative Optical Anisotropy Imaging (QOAI). A fast and precise single-particle characterizing technique for anisotropic nanostructures, QOAI allows real-time tracking of particle orientation as well as the spectroscopic characterization of polarizabilities of nanoparticles on a microsecond timescale. The abilities of QOAI are demonstrated by the detection and the characterization of single gold nanorods. We also show that single particle diffusions and the process of particle binding to a wall can be tracked through QOAI. The rotational diffusivities of gold nanorods near the wall were determined by autocorrelation analysis, which shows that the diffusivity in the polar direction is slightly smaller than in the azimuthal direction. This result demonstrates that a detailed correlation analysis with QOAI may provide the opportunity to analyze both the translational and rotational motion of particles simultaneously, enabling true 3-dimensional orientation tracking. Finally, optical methods including QOAI are applied to the investigation of magnetic assembly, demonstrating that optical anisotropy is generated during particle binding, which can be used as a probe of the magnetic assembly process. QOAI is employed to track the dynamics of magnetic clusters in real time, attempting to capture insights on the self-assembly of the magnetic nanoparticles. By turning the external magnetic field on and off, the processes of combining superparamagnetic colloidal nanoparticle clusters into chain assemblies are monitored along with the chain growth. This fast and orientation-sensitive single-particle measurement opens the door to detailed studies of self-assembly away from equilibrium.
- Surface plasmon resonance study of the purple gold (AuAl₂) intermetallic, pH-responsive fluorescence gold nanoparticles, and gold nanosphere assemblySamaimongkol, Panupon (Virginia Tech, 2018-07-31)In this dissertation, I have verified that the striking purple color of the intermetallic compound AuAl₂, also known as purple gold, originates from surface plasmons (SPs). This contrasts to a previous assumption that this color is due to an interband absorption transition. The existence of SPs was demonstrated by launching them in thin AuAl2 films in the Kretschmann configuration, which enables us to measure the SP dispersion relation. I observed that the SP energy in thin films of purple gold is around 2.1 eV, comparable to previous work on the dielectric function of this material. Furthermore, SP sensing using AuAl₂ also shows the ability to measure the change in the refractive index of standard sucrose solution. AuAl₂ in nanoparticle form is also discussed in terms of plasmonic applications, where Mie scattering theory predicts that the particle bears nearly uniform absorption over the entire visible spectrum with an order magnitude higher than a lightabsorbing carbonaceous particle. The second topic of this dissertation focuses on plasmon enhanced fluorescence in gold nanoparticles (Au NPs). Here, I investigated the distance-dependent fluorescence emission of rhodamine green 110 fluorophores from Au NPs with tunable spacers. These spacers consist of polyelectrolyte multilayers (PEMs) consisting of poly(allylamine hydrochloride) and poly(styrene sulfonate) assembled at pH 8.4. The distance between Au NPs and fluorophores was varied by changing the ambient pH from 3 to 10 and back, which causes the swelling and deswelling of PEM spacer. Maximum fluorescence intensity with 4.0-fold enhancement was observed with 7-layer coated Au NPs at ambient pH 10 referenced to pH 3. The last topic of this dissertation examines a novel approach to assemble nanoparticles, in particular, dimers of gold nanospheres (NSs). 16 nm and 60 nm diameter NSs were connected using photocleavable molecules as linkers. I showed that the orientation of the dimers can be controlled with the polarization of UV illumination that cleaves the linkers, making dipolar patches. This type of assembly provides a simple method with potential applications in multiple contexts, such as biomedicine and nanorobotics.
- Temperature and Doping-Dependent Interplay between Direct and Indirect Optical Response in Buffer-Mediated Epitaxial GermaniumHudait, Mantu K.; Meeker, Michael; Liu, Jheng-Sin; Clavel, Michael; Bhattacharya, Shuvodip; Khodaparast, Giti (Elsevier, 2022-09-01)The structural and optical properties of buffer mediated epitaxial germanium (Ge) layer were investigated and compared with bulk n-type and p-type Ge substrates. An interconnected dual-chamber molecular beam epitaxy (MBE) system was used to grow a 280 nm thin Ge epilayer on (100)GaAs substrate with an intermediate AlAs buffer layer. The lattice-matched, abrupt Ge/AlAs heterointerface was analyzed using cross-sectional transmission electron microscopic analysis, and no elemental interdiffusion was detected via secondary ion mass spectrometry. A strong direct gap transition, compared to the indirect gap transition, and a series of phonon-assisted transitions was observed by photoluminescence (PL) spectroscopy. In addition, the intensity of the direct gap recombination decreases with decreasing PL measurement temperatures, which was ascribed to the reduced density of Γ-valley electrons available for recombination at lower temperature. Furthermore, the intensity ratio between the direct and indirect optical transition drastically decreases with decreasing temperature in both n-type epitaxial and p-type bulk Ge. An empirical relation in both direct and indirect peak position with temperature was established. The observed strong luminescence in 280 nm thick epitaxial Ge at room temperature is vital for Ge-based photonic devices. In addition, the quality of the epitaxial Ge layer grown via MBE is on par with bulk Ge substrates.
- Theoretical Study of Semiconductor Quantum Dot Lasers with Asymmetric Barrier LayersMonk, John Lawrence III (Virginia Tech, 2020-05-21)Small-signal dynamic response of semiconductor quantum dot (QD) lasers with asymmetric barrier layers was studied. Semiconductor lasers are used in many communication systems. Fiber optic communication systems use semiconductor lasers in order to transmit information. DVD and Blu-ray disk players feature semiconductor lasers as their readout source. Barcode readers and laser pointers also use semiconductor lasers. A medical application of semiconductor lasers is for minor soft tissue procedures. Semiconductor lasers are also used to pump solid-state and fiber lasers. Semiconductor lasers are able to transmit telephone, internet, and television signals through fiber optic cables over long distances. The amount of information able to be transferred is directly related to the bandwidth of the laser. By introducing asymmetric barrier layers, the modulation bandwidth of the laser will improve, allowing for more information to be transferred. Also, by introducing asymmetric barrier layers, the output power will be unrestricted, meaning as more current is applied to the system, the laser will get more powerful. An optimum pumping current was found which maximized modulation bandwidth at -3dB, and is lower in QD lasers with asymmetric barrier layers (ABL) as opposed to conventional QD lasers. Modulation bandwidth was found to increase with cross section of carrier capture before reaching an asymptote. Both surface density of QDs and cavity length had optimum values which maximized modulation bandwidth. Relative QD size fluctuation was considered in order to see how variation in QD sizes effects the modulation bandwidth of the semiconductor QD laser with ABLs. These calculations give a good starting point for fabricating semiconductor QD lasers with ABLs featuring the largest modulation bandwidth possible for fiber optic communication systems. In semiconductor QD lasers, the electrons and holes may be captured into excited states within the QDs, rather than the ground state. The particles may also jump from the ground state up to an excited state, or drop from the excited state to the ground state. Recombination of electron-hole pairs can occur from the ground state to the ground state or from an excited state to an excited state. In the situation if the capture of charge carriers into the ground state in QDs takes place via the excited-state, then this two-step capture process makes the output power from ground-state lasing to saturate in conventional QD lasers. By using ABLs in the QD laser, it is predicted that the output power of ground-state lasing will continue to rise with applied current, as the ABLs will stop the electrons and holes from recombining in the optical confinement layer. Thus, ABL QD lasers will be able to be used in applications that require large energy outputs.