Few-layer black phosphorous (FLBP) is one of the most important two-dimensional (2D) materials due to its strongly layer-dependent quantized bandstructure, which leads to wavelength-tunable optical and electrical properties. This thesis focuses on the preparation of stable, high-quality FLBP, the characterization of its optical properties, and device applications.Part I presents an approach to preparing high-quality, stable FLBP samples by combining O2 plasma etching, boron nitride (BN) sandwiching, and subsequent rapid thermal annealing (RTA). Such a strategy has successfully produced FLBP samples with a record-long lifetime, with 80% of photoluminescence (PL) intensity remaining after 7 months. The improved material quality of FLBP allows the establishment of a more definitive relationship between the layer number and PL energies. Part II presents the study of oxygen incorporation in FLBP. The natural oxidation formed in the air environment is dominated by the formation of interstitial oxygen and dangling oxygen. By the real-time PL and Raman spectroscopy, it is found that continuous laser excitation breaks the bonds of interstitial oxygen, and free oxygen atoms can diffuse around or form dangling oxygen under low heat. RTA at 450 °C can turn the interstitial oxygen into dangling oxygen more thoroughly. Such oxygen-containing samples show similar optical properties to the pristine BP samples. The bandgap of such FLBP samples increases with the concentration of the incorporated oxygen. Part III deals with the investigation of emission natures of the prepared samples. The power- and temperature-dependent measurements demonstrate that PL emissions are dominated by excitons and trions, with a combined percentage larger than 80% at room temperature. Such measurements allow the determination of trion and exciton binding energies of 2-, 3-, and 4-layer BP, with values around 33, 23, 15 meV for trions and 297, 276, 179 meV for excitons at 77K, respectively. Part IV presents the initial exploration of device applications of such FLBP samples. The coupling between photonic crystal cavity (PCC) modes and FLBP's emission is realized by integrating the prepared sandwich structure onto 2D PCC. Electroluminescence has also been achieved by integrating such materials onto interdigital electrodes driven by alternating electric fields.

Optical metasurfaces, i.e. artificially engineered arrays of subwavelength building blocks supporting abrupt and substantial light confinement, was employed to demonstrate a novel generation of devices for circularly polarized detection, full-Stokes polarimetry and all-optical modulation with ultra-compact footprint and chip-integrability.

Optical chirality is essential for generation, manipulation and detection of circularly polarized light (CPL), thus finds many applications in quantum computing, communication, spectroscopy, biomedical diagnosis, imaging and sensing. Compared to natural chiral materials, chiral metamaterials and metasurfaces enable much stronger chirality on subwavelength scale; therefore, they are ideal for device miniaturization and system integration. However, they are usually associated with low performance due to limited fabrication tolerance and high dissipation mainly caused by plasmonic materials. Here, a bio-inspired submicron-thick chiral metamaterial structure was designed and demonstrated experimentally with high contrast (extinction ratio >35) detection of CPL with different handedness and high efficiency (>80%) of the overall device. Furthermore, integration of left- and right-handed CPL detection units with nanograting linear polarization filters enabled full-Stokes polarimetry of arbitrarily input polarization states with high accuracy and very low insertion loss, all on a submillimeter single chip. These unprecedented highly efficient and high extinction ratio devices pave the way for on-chip polarimetric measurements.

All-optical modulation is widely used for optical interconnects, communication, information processing, and ultrafast spectroscopy. Yet, there’s deficiency of ultrafast, compact and energy-efficient solutions all in one device. Here, all-optical modulation of light in the near- and mid-infrared regimes were experimentally demonstrated based on a graphene-integrated plasmonic nanoantenna array. The remarkable feature of the device design is its simultaneous near-field enhancement for pump and probe (signal) beams, owing to the localized surface plasmon resonance excitation, while preserving the ultrafast photocarrier relaxation in graphene. Hence, a distinct modulation at 1560nm with record-low pump fluence (<8μJ/cm^2) was reported with ~1ps response time. Besides, relying on broadband interaction of graphene with incident light, a first-time demonstration of graphene-based all-optical modulation in mid-infrared spectral region (6-7μm) was reported based on the above double-enhancement design concept. Relying on the tunability of metasurface design, the proposed device can be used for ultrafast optical modulation from near-infrared to terahertz regime.

Photonic integrated circuit (PIC) in the visible spectrum opens up new opportunities for frequency metrology, neurophotonics, and quantum technologies. Group III nitride (III-N) compound semiconductor is a new emerging material platform for PIC in visible spectrum. The ultra-wide bandgap of aluminum nitride (AlN) allows broadband transparency. The high quantum efficiency of indium gallium nitride (InGaN) quantum well is the major enabler for solid-state lighting and provides the opportunities for active photonic integration. Additionally, the two-dimensional electron gas induced by spontaneous and polarization charges within III-N materials exhibit large electron mobility, which is promising for the development of high frequency transistors. Moreover, the noncentrosymmetric crystalline structure gives nonzero second order susceptibility, beneficial for the application of second harmonic generation and entangled photon generation in nonlinear and quantum optical technologies. Despite the promising features of III-N materials, the investigations on the III-N based PICs are still primitive, mainly due to the difficulties in material growth and the lack of knowledge on fundamental material parameters. In this work, firstly, the fundamental nonlinear optical properties of III-N materials will be characterized. Then, the fabrication process flow of III-N materials will be established. Thirdly, the waveguide performance will be theoretically and experimentally evaluated. At last, the supercontinuum generation from visible to infrared will be demonstrated by utilizing soliton dynamics in high order guided modes. The outcome from this work paves the way towards fully integrated optical comb in UV and visible spectrum.

The larger tolerance to lattice mismatch in growth of semiconductor nanowires (NWs) offers much more flexibility for achieving a wide range of compositions and bandgaps via alloying within a single substrate. The bandgap of III-V InGaAsP alloy NWs can be tuned to cover a wide range of (0.4, 2.25) eV, appealing for various optoelectronic applications such as photodetectors, solar cells, Light Emitting Diodes (LEDs), lasers, etc., given the existing rich knowledge in device fabrication based on these materials.

This dissertation explores the growth of InGaAsP alloys using a low-cost method that could be potentially important especially for III-V NW-based solar cells. The NWs were grown by Vapor-Liquid-Solid (VLS) and Vapor-Solid (VS) mechanisms using a Low-Pressure Chemical Vapor Deposition (LPCVD) technique. The concept of supersaturation was employed to control the morphology of NWs through the interplay between VLS and VS growth mechanisms. Comprehensive optical and material characterizations were carried out to evaluate the quality of the grown materials.

The growth of exceptionally high quality III-V phosphide NWs of InP and GaP was studied with an emphasis on the effects of vastly different sublimation rates of the associated III and V elements. The incorporation of defects exerted by deviation from stoichiometry was examined for GaP NWs, with an aim towards maximization of bandedge-to-defect emission ratio. In addition, a VLS-VS assisted growth of highly stoichiometric InP thin films and nano-networks with a wide temperature window from 560◦C to 720◦C was demonstrated. Such growth is shown to be insensitive to the type of substrates such as silicon, InP, and fused quartz. The dual gradient method was exploited to grow composition-graded ternary alloy NWs of InGaP, InGaAs, and GaAsP with different bandgaps ranging from 0.6 eV to 2.2 eV, to be used for making laterally-arrayed multiple bandgap (LAMB) solar cells. Furthermore, a template-based growth of the NWs was attempted based on the Si/SiO2 substrate. Such platform can be used to grow a wide range of alloy nanopillar materials, without being limited by typical lattice mismatch, providing a low cost universal platform for future PV solar cells.

Light Emitting Diodes even with their longer life, robust build and low power consumption, they are still plagued by some problems the most significant of which are the current droop and thermal droop. Current droop causes a lowering in the Internal Quantum Efficiency with increased current injection while thermal droop lowers the whole Internal Quantum Efficiency curve with increase in temperature. The focus here was understanding effects of thermal droop and develop a method to control it.

Shockley Read Hall recombination plays a dominant role in the thermal droop effect when the current injection is low. Since the blue light emitting diode is based on Gallium Nitride, we need to take into consideration the effect of piezoelectric polarization in the quantum wells. The effects of the piezoelectric fields were studied based on the Gallium Nitride plane orientations. It was found in a Gallium Nitride light emitting diodes simulation study that more the number of quantum wells, lower would be the Radiative recombination rate. The problem of exacerbated spatial separation of electron hole wavefunctions in a thick single quantum well structure lead to the development of a dual well structure where one well assisted the other during high temperature operations. The Electron Blocking Layer was reduced in thickness and was made only 10 nm thick with a 5 nm Gallium Nitride buffer between it and the active region wells. The main reason for reducing the electron blocking layer thickness was to reduce the valance band offset and improve hole transport into the active region. Three different dual well designs were simulated of 3nm, 6nm and 9nm wide wells. The output parameters like the Power Spectral Density, Electron bound density, Light Output Power and Electron-Hole wavefunction overlaps were calculated. It was found that one of the wells acted as an assisting well where it had very little radiative recombination activity in it at room temperature.

As the temperature increased, it was observed that the electrons in the main well started to overflow out of it and into the assisting well where the radiative recombination rate increased significantly. This lead to a boost in Internal Quantum Efficiency.

This dissertation aims to study and understand the effect of nonlinear dynamics and quantum chaos in graphene, optomechanics, photonics and spintronics systems.

First, in graphene quantum dot systems, conductance fluctuations are investigated from the respects of Fano resonances and quantum chaos. The conventional semi-classical theory of quantum chaotic scattering used in this field depends on an invariant classical phase-space structure. I show that for systems without an invariant classical phase-space structure, the quantum pointer states can still be used to explain the conductance fluctuations. Another finding is that the chaotic geometry is demonstrated to have similar effects as the disorders in transportations.

Second, in optomechanics systems, I find rich nonlinear dynamics. Using the semi-classical Langevin equations, I demonstrate a quasi-periodic motion is favorable for the quantum entanglement between the optical mode and mechanical mode. Then I use the quantum trajectory theory to provide a new resolution for the breakdown of the classical-quantum correspondences in the chaotic regions.

Third, I investigate the analogs of the electrical band structures and effects in the non-electrical systems. In the photonic systems, I use an array of waveguides to simulate the transport of the massive relativistic particle in a non-Hermitian scenario. A new form of Zitterbewegung is discovered as well as its analytical explanation. In mechanical systems, I use springs and mass points systems to achieve a three band degenerate band structure with a new pair of spatially separated edge states in the Dice lattice. A new semi-metal phase with the intrinsic valley-Hall effect is found.

At last, I investigate the nonlinear dynamics in the spintronics systems, in which the topological insulator couples with a magnetization. Rich nonlinear dynamics are discovered in this systems, especially the multi-stability states.

Semiconductor nanolasers, as a frontier subject has drawn a great deal of attention over the past decade. Semiconductor nanolasers are compatible with on-chip integrations towards the ultimate realization of photonic integrated circuits. However, innovative approaches are strongly required to overcome the limitation of lattice-mismatch issues. In this dissertation, two alternative approaches are employed to overcome the lattice-mismatch issues. i) By taking advantage of nanowires or nanobelts techniques, flexibility in bandgap engineering has been greatly expanded, resulting in the nanolasers with wide wavelength coverage and tunability. Simultaneous two-color lasing in green and red is firstly achieved from monolithic cadmium sulfide selenide nanosheets. The wavelength separation is up to 97 nm at room temperature, larger than the gain bandwidth of a single semiconductor material in the visible wavelength range. The strategies adopted for two-color lasers eventually leads to the realization of simultaneous red, green and blue lasing and white lasing from a single zinc cadmium sulfide selenide nanosheet with color tunability in the full visible range, making a major milestone in the ultimate solution of laser illumination and laser display. In addition, with the help of nanowire techniques, material emission has been extended to mid-infrared range, enabling lasing at ~3µm from single lead sulfide subwavelength wires at 180 K. The cavity volume of the subwavelength laser is down to 0.44 λ3 and the wavelength tuning range is over 270 nm through the thermo-optic mechanism, exhibiting considerable potentials for on-chip applications in mid-infrared wavelength ranges. ii) By taking advantage of membrane transfer techniques, heterogeneous integration of compound semiconductor and waveguide material becomes possible, enabling the successful fabrication of membrane based nano-ring lasers on a dielectric substrate. Thin membranes with total thickness of ~200nm are first released from the original growth substrate and then transferred onto a receiving substrate through a generally applicable membrane transfer method. Nano-ring arrays are then defined by photolithography with an individual radius of 750 nm and a radial thickness of 400-500 nm. As a result, single mode lasing is achieved on individual nano-ring lasers at ~980 nm with cavity volumes down to 0.24 λ3, providing a general avenue for future heterogeneous integration of nanolasers on silicon substrates.

Nanowires are 1D rod-like structures which are regarded as the basis for future technologies. III-V nanowires have attracted immense attention because of their stability, crystal quality and wide use. In this work, I focus on the growth and characterization of III-V semiconductor nanowires, in particular GaP, InP and InGaP alloys. These nanowires were grown using a hot wall CVD(Chemical Vapor Deposition) setup and are characterized using SEM (Scanning Electron Microscope), EDX (Energy Dispersive X-ray Spectroscopy) and PL (Photoluminescence) techniques.



In the first chapter, Indium Phosphide nanowires were grown using elemental sources (In and P powders). I consider the various kinds of InP morphologies grown using this method. The effect of source temperature on the stoichiometry and optical properties of nanowires is studied. Lasing behavior has been seen in InP nanostructures, showing superior material quality of InP.

InGaP alloy nanowires were grown using compound and elemental sources. Nanowires grown using compound sources have significant oxide incorporation and showed kinky morphology. Nanowires grown using elemental sources had no oxide and showed better optical quality. Also, these samples showed a tunable alloy composition across the entire substrate covering more than 50% of the InGaP alloy system. Integrated intensity showed that the bandgap of the nanowires changed from indirect to direct bandgap with increasing Indium composition. InGaP alloy nanowires were compared with Gallium Phosphide nanowires in terms of PL emission, using InGaP nanowires it is possible to grow nanowires free of defects and oxygen impurities, which are commonly encountered in GaP nanowires.

To detect and resolve sub-wavelength features at optical frequencies, beyond the diffraction limit, requires sensors that interact with the electromagnetic near-field of those features. Most instruments operating in this modality scan a single detector element across the surface under inspection because the scattered signals from a multiplicity of such elements would end up interfering with each other. However, an alternative massively parallelized configuration, consisting of a remotely interrogating array of dipoles, capable of interrogating multiple adjacent areas of the surface at the same time, was proposed in 2002.

In the present work a remotely interrogating slot antenna inside a 60nm silver slab is designed which increases the signal to noise ratio of the original system. The antenna is tuned to resonance at 600nm range by taking advantage of the plasmon resonance properties of the metal’s negative permittivity and judicious shaping of the slot element. Full-physics simulations show the capability of detecting an 8nm particle using red light illumination. The sensitivity to the λ/78 particle is attained by detecting the change induced on the antenna’s far field signature by the proximate particle, a change that is 15dB greater than the scattering signature of the particle by itself.

To verify the capabilities of this technology in a readily accessible experimental environment, a radiofrequency scale model is designed using a meta-material to mimic the optical properties of silver in the 2GHz to 5GHz range. Various approaches to the replication of the metal’s behavior are explored in a trade-off between fidelity to the metal’s natural plasmon response, desired bandwidth of the demonstration, and

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manufacturability of the meta-material. The simulation and experimental results successfully verify the capability of the proposed near-field sensor in sub-wavelength detection and imaging not only as a proof of concept for optical frequencies but also as a potential imaging device for radio frequencies.

Nanowires are one-dimensional (1D) structures with diameter on the nanometer scales with a high length-to-diameter aspect ratio. Nanowires of various materials including semiconductors, dielectrics and metals have been intensively researched in the past two decades for applications to electrical and optical devices. Typically, nanowires are synthesized using the vapor-liquid-solid (VLS) approach, which allows defect-free 1D growth despite the lattice mismatch between nanowires and substrates. Lattice mismatch issue is a serious problem in high-quality thin film growth of many semiconductors and non-semiconductors. Therefore, nanowires provide promising platforms for the applications requiring high crystal quality materials.

With the 1D geometry, nanowires are natural optical waveguides for light guiding and propagation. By introducing feedback mechanisms to nanowire waveguides, such as the cleaved end facets, the nanowires can work as ultra-small size lasers. Since the first demonstration of the room-temperature ultraviolet nanowire lasers in 2001, the nanowire lasers covering from ultraviolet to mid infrared wavelength ranges have been intensively studied. This dissertation focuses on the optical characterization and laser fabrication of two nanowire materials: erbium chloride silicate nanowires and composition-graded CdSSe semiconductor alloy nanowires.

Chapter 1 – 5 of this dissertation presents a comprehensive characterization of a newly developed erbium compound material, erbium chloride silicate (ECS) in a nanowire form. Extensive experiments demonstrated the high crystal quality and excellent optical properties of ECS nanowires. Optical gain higher than 30 dB/cm at 1.53 μm wavelength is demonstrated on single ECS nanowires, which is higher than the gain of any reported erbium materials. An ultra-high Q photonic crystal micro-cavity is designed on a single ECS nanowire towards the ultra-compact lasers at communication wavelengths. Such ECS nanowire lasers show the potential applications of on-chip photonics integration.

Chapter 6 – 7 presents the design and demonstration of dynamical color-controllable lasers on a single CdSSe alloy nanowire. Through the defect-free VLS growth, engineering of the alloy composition in a single nanowire is achieved. The alloy composition of CdSxSe1-x uniformly varies along the nanowire axis from x=1 to x=0, giving the opportunity of multi-color lasing in a monolithic structure. By looping the wide-bandgap end of the alloy nanowire through nanoscale manipulation, the simultaneous two-color lasing at green and red colors are demonstrated. The 107 nm wavelength separation of the two lasing colors is much larger than the gain bandwidth of typical semiconductors. Since the two-color lasing shares the output port, the color of the total lasing output can be controlled dynamically between the two fundamental colors by changing the relative output power of two lasing colors. Such multi-color lasing and continuous color tuning in a wide spectral range would eventually enable color-by-design lasers to be used for lighting, display and many other applications.