Dynamic Nanoplasmonics

Light can strongly interact with metallic nanostructures, leading collective oscillations of conduction electrons known as particle plasmons. For a long time, gold and silver have been the metals of choice for constructing plasmonic nanodevices, given their excellent optical properties. However, these metals present static optical responses. In the past decade, tremendous interest has been witnessed in dynamically controlling the optical properties of plasmonic nanostructures. To enable dynamic functionality, several approaches have been proposed and implemented. First one is to manipulate the configurations of plasmonic structures. Second one is to tune the dielectric surroundings of plasmonic nanostructures. Third one, which is probably the most intriguing one, is to directly regulate the carrier densities and dielectric functions of the metals themselves. Magnesium is one of the promising candidates, as it exhibits excellent optical properties at high frequencies and can absorb/desorb hydrogen, undergoing reversible transitions between metal and dielectric hydride states. This offers great opportunities to design and construct dynamic optical nanodevices at visible frequencies. We envision that Magnesium-based dynamic nanoplasmonics will not only provide insights into understanding the catalytic processes of hydrogen diffusion in metals on the nanometer scale by optical means but also it will open an avenue towards functional plasmonic nanodevices with tailored optical properties for real-world applications

Organic lasers: recent developments on materials, device geometries, and fabrication techniques

MCG acknowledges financial support through the ERC Starting Grant ABLASE (640012) and the European Union Marie Curie Career Integration Grant (PCIG12-GA-2012-334407). AJCK acknowledges financial support by the German Federal Ministry for Education and Research through a NanoMatFutur research group (BMBF grant no. 13N13522).Organic dyes have been used as gain medium for lasers since the 1960s, long before the advent of today’s organic electronic devices. Organic gain materials are highly attractive for lasing due to their chemical tunability and large stimulated emission cross section. While the traditional dye laser has been largely replaced by solid-state lasers, a number of new and miniaturized organic lasers have emerged that hold great potential for lab-on-chip applications, biointegration, low-cost sensing and related areas, which benefit from the unique properties of organic gain materials. On the fundamental level, these include high exciton binding energy, low refractive index (compared to inorganic semiconductors), and ease of spectral and chemical tuning. On a technological level, mechanical flexibility and compatibility with simple processing techniques such as printing, roll-to-roll, self-assembly, and soft-lithography are most relevant. Here, the authors provide a comprehensive review of the developments in the field over the past decade, discussing recent advances in organic gain materials, which are today often based on solid-state organic semiconductors, as well as optical feedback structures, and device fabrication. Recent efforts toward continuous wave operation and electrical pumping of solid-state organic lasers are reviewed, and new device concepts and emerging applications are summarized.PostprintPeer reviewe

Bio-Inspired Nanomembranes as Building Blocks for Nanophotonics, Plasmonics and Metamaterials

Nanomembranes are the most widespread building block of life, as they encompass cell and organelle walls. Their synthetic counterparts can be described as freestanding or free-floating structures thinner than 100 nm, down to monatomic/monomolecular thickness and with giant lateral aspect ratios. The structural confinement to quasi-2D sheets causes a multitude of unexpected and often counterintuitive properties. This has resulted in synthetic nanomembranes transiting from a mere scientific curiosity to a position where novel applications are emerging at an ever-accelerating pace. Among wide fields where their use has proven itself most fruitful are nano-optics and nanophotonics. However, the authors are unaware of a review covering the nanomembrane use in these important fields. Here, we present an attempt to survey the state of the art of nanomembranes in nanophotonics, including photonic crystals, plasmonics, metasurfaces, and nanoantennas, with an accent on some advancements that appeared within the last few years. Unlimited by the Nature toolbox, we can utilize a practically infinite number of available materials and methods and reach numerous properties not met in biological membranes. Thus, nanomembranes in nano-optics can be described as real metastructures, exceeding the known materials and opening pathways to a wide variety of novel functionalities

MEMS tunable infrared metamaterial and mechanical sensors

Sub-wavelength resonant structures open the path for fine controlling the near-field at the nanoscale dimension. They constitute into macroscopic “metamaterials” with macroscale properties such as transmission, reflection, and absorption being tailored to exhibit a particular electromagnetic response. The properties of the resonators are often fixed at the time of fabrication wherein the tunability is demanding to overcome fabrication tolerances and afford fast signal processing. Hybridizing dynamic components such as optically active medium into the device makes tunable devices. Microelectromechanical systems (MEMS) compatible integrated circuit fabrication process is a promising platform that can be merged with photonics or novel 2D materials. The prospect of enormous freedom in integrating nanophotonics, MEMS actuators and sensors, and microelectronics into a single platform has driven the rapid development of MEMS-based sensing devices. This thesis describes the design and development of four tunable plasmonic structures based on active media or MEMS, two graphene-based MEMS sensors and a novel tape-based cost-effective nanotransfer printing techniques. First of all, we present two tunable plasmonic devices with the use of two active medium, which are electrically controlled liquid crystals and temperature-responsive hydrogels, respectively. By incorporating a nematic liquid crystal layer into quasi-3D mushroom plasmonic nanostructures and thanks to the unique coupling between surface plasmon polariton and Rayleigh anomaly, we have achieved the electrical tuning of the properties of plasmonic crystal at a low operating electric field. We also present another tunable plasmonic device with the capability to sense environmental temperature variations. The device is bowtie nanoantenna arrays coated with a submicron-thick, thermos-responsive hydrogel. The favorable scaling of plasmonic dimers at the nanometer scale and ionic diffusion at the submicron scale is leveraged to achieve strong optical resonance and rapid hydrogel response, respectively. Secondly, we present two MEMS -based tunable near-to-mid infrared metamaterials on a silicon-on-insulator wafer via electrically and thermally actuating the freestanding nanocantilevers. The two devices are developed on the basis of the same fabrication process and are easy-to-implement. The electrostatically driven metamaterial affords ultrahigh mechanical modulation (several tens of MHz) of an optical signal while the thermo-mechanically tunable metamaterial provides up to 90% optical signal modulation at a wavelength of 3.6 õm. Next, we present MEMS graphene-based pressure and gas flow sensors realized by transferring a large area and few-layered graphene onto a suspended silicon nitride thin membrane perforated with micro-through-holes. Due to the increased strain in the through-holes, the pressure sensor exhibits a very high sensitivty outperformed than most existing MEMS-based pressure sensors using graphene, silicon, and carbon nanotubes. An air flow sensor is also demonstrated via patterning graphene sheets with flow-through microholes. The flow rate of the air is measured by converting the mechanically deflection of the membrane into the electrical readout due to the graphene piezeroresistors. Finally, we present a tape-based multifunctional nanotransfer printing process based on a simple stick-and-peel procedure. It affords fast production of large-area metallic and dielectric nanophotonic sensing devices and metamaterials using Scotch tape

Novel Materials and Devices for Terahertz Detection and Emission for Sensing, Imaging and Communication

Technical advancement is required to attain a high data transmission rate, which entails expanding beyond the currently available bandwidth and establishing a new standard for the highest data rates, which mandates a higher frequency range and larger bandwidth. The THz spectrum (0.1-10 THz) has been considered as an emerging next frontier for the future 5G and beyond technology. THz frequencies also offer unique characteristics, such as penetrating most dielectric materials like fabric, plastic, and leather, making them appealing for imaging and sensing applications. Therefore, employing a high-power room temperature, tunable THz emitters, and a high responsivity THz detector is essential. Dyakonov-theory Shur\u27s was applied in this dissertation to achieve tunable THz detection and emission by plasma waves in high carrier density channels of field-effect devices. The first major contribution of this dissertation is developing graphene-based THz plasmonics detector with high responsivity. An upside-down free-standing graphene in a field effect transistor based resonant room temperature THz detector device with significantly improved mobility and gate control has been presented. The highest achieved responsivity is ~3.1kV/W, which is more than 10 times higher than any THz detector reported till now. The active region is predominantly single-layer graphene with multi-grains, even though the fabricated graphene THz detector has the highest responsivity. The challenges encountered during the fabrication and measurement of the graphene-based detector have been described, along with a strategy to overcome them while preserving high graphene mobility. In our new design, a monolayer of hBN underneath the graphene layer has been deposited to increase the mobility and electron concentration rate further. We also investigated the diamond-based FETs for their potential characteristics as a THz emitters and detectors. Diamond\u27s wide bandgap, high breakdown field, and high thermal conductivity attributes make it a potential semiconductor material for high voltage, high power, and high-temperature operation. Diamond is a good choice for THz and sub-THz applications because of its high optical phonon scattering and high momentum relaxation time. Numerical and analytical studies of diamond materials, including p-diamond and n-diamond materials, are presented, indicating their effectiveness as a prospective contender for high temperature and high power-based terahertz applications These detectors are expected to be a strong competitor for future THz on-chip applications due to their high sensitivity, low noise, tunability, compact size, mobility, faster response time, room temperature operation, and lower cost. Furthermore, when plasma wave instabilities are induced with the proper biasing, the same devices can be employed as THz emitters, which are expected to have a higher emission power. Another key contribution is developing a method for detecting counterfeit, damaged, forged, or defective ICs has been devised utilizing a new non-destructive and unobtrusive terahertz testing approach to address the crucial point of hardware cybersecurity and system reliability. The response of MMICs, VLSI, and ULSIC to incident terahertz and sub-terahertz radiation at the circuit pins are measured and analyzed using deep learning. More sophisticated terahertz response profiles and signatures of specific ICs can be created by measuring a more significant number of pins under different frequencies, polarizations, and depth of focus. The proposed method has no effect on ICs operation and could provide precise ICs signatures. The classification process between the secure and unsecure ICs images has been explained using data augmentation and transfer learning-based convolution neural network with ~98% accuracy. A planar nanomatryoshka type core-shell resonator with hybrid toroidal moments is shown both experimentally and analytically, allowing unique characteristics to be explored. This resonator may be utilized for accurate sensing, immunobiosensing, quick switching, narrow-band filters, and other applications

MANIPULATION OF LIGHT VIA SUBWAVELENGTH NANOSTRUCTURES

Ph.DDOCTOR OF PHILOSOPH

Twisted van der Waals Quantum Materials: Fundamentals, Tunability and Applications

Twisted vdW quantum materials have emerged as a rapidly developing field of 2D semiconductors. These materials establish a new central research area and provide a promising platform for studying quantum phenomena and investigating the engineering of novel optoelectronic properties such as single-photon emission, non-linear optical response, magnon physics, and topological superconductivity. These captivating electronic and optical properties result from, and can be tailored by, the interlayer coupling using moir\'e patterns formed by vertically stacking atomic layers with controlled angle misorientation or lattice mismatch. Their outstanding properties and the high degree of tunability position them as compelling building blocks for both compact quantum-enabled devices and classical optoelectronics. This article offers a comprehensive review of recent advancements in the understanding and manipulation of twisted van der Waals structures and presents a survey of the state-of-the-art research on moir\'e superlattices, encompassing interdisciplinary interests. It delves into fundamental theories, synthesis and fabrication, and visualization techniques, and the wide range of novel physical phenomena exhibited by these structures, with a focus on their potential for practical device integration in applications ranging from quantum information to biosensors, and including classical optoelectronics such as modulators, light emitting diodes (LEDs), lasers, and photodetectors. It highlights the unique ability of moir\'e superlattices to connect multiple disciplines, covering chemistry, electronics, optics, photonics, magnetism, topological and quantum physics. This comprehensive review provides a valuable resource for researchers interested in moir\'e superlattices, shedding light on their fundamental characteristics and their potential for transformative applications in various fields.Comment: 179 pages, 42 figures, Chemical Review

Tunable multiscale infrared plasmonics with metal oxide nanocrystals

Degenerately doped semiconductor nanocrystals (NC) exhibit a localized surface plasmon resonance (LSPR) that falls in the near- to mid-IR range of the electromagnetic spectrum. Unlike metal, the metal oxide LSPR characteristics can be further tuned by doping, and structural control, or by in situ electrochemical or photochemical charging. Here, we illustrate how intrinsic NC attributes like its crystal structure, shape and size, along with band structure and surface properties affects the LSPR properties and its possible applications. First, the interplay of NC shape and the intrinsic crystal structure on the LSPR was studied using model systems of In:CdO and Cs:WO₃, the latter of which has an intrinsic anisotropic crystal structure. For both systems, a change of shape from spherical to faceted NCs led to as anticipated higher near field enhancements around the particle. However, with Cs:WO₃, presence of an anisotropic hexagonal crystal structure, leads to additional strong LSPR band-splitting into two distinct peaks with comparable intensities. Second, plasmon-molecular vibration coupling, as a proof of concept for sensing applications, was shown using newly developed F and Sn codoped In₂O₃ NCs to couple to the C-H vibration of surface-bound oleate ligands. A combined theoretical and experimental approach was employed to describe the observed plasmon-plasmon coupling, the influence of coupling strength and relative detuning between the molecular vibration and LSPR on the enhancement factor, and the observed Fano lineshape by deconvoluting the combined response of the LSPR and molecular vibration in transmission, absorption, and reflection. Third, plasmon modulation through dynamic carrier density tuning was investigated using thin films of monodisperse ITO NCs with various doping level and sizes along with an in situ electrochemical setup. From the combination of the in-situ spectroelectrochemical analysis and optical modeling, it was found that often-neglected semiconductor properties, such as band structure modification upon doping and surface chemistry, strongly affect the LSPR modulation behavior. The influence of band structure and effects like Fermi level pinning by surface defect states were shown to cause a surface depletion layer that alters the LSPR properties, namely the extent of LSPR modulation, near field enhancement, and sensitivity of the LSPR to the surrounding.Chemical Engineerin