Theses supervised by Doç. Dr. Hilmi Volkan Demir

Yüksek verimli indüktif bobin dizinleri

Inductive heating is widely exploited in industrial operations including metal hardening, forging and brazing. Recently, as a promising alternative to traditional heating, inductive heating has attracted substantial commercial interest for domestic cookers. This is because inductive heating offers fast, precise and efficient heating compared to traditional methods that make use of either convection or conduction as a means of heat transfer. To introduce full flexibility in using the cooking space, a strong demand is currently directed toward all-surface induction ovens, with the capability to heat a vessel placed arbitrarily anywhere on the surface of the induction cook top. For this purpose, inductive coils of tens of mm in diameter are required to be designed and stacked together to form coil arrays. However, this typically comes at the cost of reduced efficiency. To address this problem, this thesis work focuses on high-efficiency coil arrays designed for all-surface induction with optimum ferrite placement. The thesis work proposes and demonstrates unique coil geometry and array stacking that utilizes mutual coupling between the coils for substantially increased efficiency. Here analytical, numerical and experimental electromagnetic analyses of sample coils are performed. Effects of different ferrite placements are investigated and, contrary to the general intuition of placing ferrite bars only under the coil, an effective way of ferrite placement is proposed and shown. These results indicate that the proposed high-efficiency arrays of inductive coils are highly promising for all-surface inductive heating.

Yüksek polarize ışıma, saçılma ve algılama için solüsyon bazlı işlenmiş nanoyapılar ve aygıtlar

Recent advancements in photonics have facilitated robust and reliable light sources, displays and photosensors with relatively long lifetimes and high energy efficiency in their classes. However, developing intrinsically polarization selective photonic devices still remains a challenge, although polarization sensitivity is essential to various advanced functions and/or improved performance. One of the main difficulties in making such devices emerges from the compromise on the efficiency while striving to reach high polarization contrast levels. For instance, commercially available birefringent structures including those integrating liquid crystals suffer from major transmission losses. On the other hand, solution-processed, high aspect-ratio nanostructures may offer power efficient platforms with high polarization contrasts via selection of the polarization in a preferred direction during emission, absorption and/or scattering process(es) while suppressing efficiency of the relevant ones in the other polarization. In this thesis, we present solution-processed metal and semiconductor nanostructures and optoelectronic devices made from them for highly polarized light generation and enhanced photosensing. Here we developed and demonstrated in-template fabricated suspended arrays of plasmonic thin nanodiscs with tunable disc-heights and gap-widths tailoring absorption and scattering properties for applications ranging from polarized light scattering to photodetection. Also, we proposed and showed highly polarized light emission in coupled thin films of magnetically aligned multi-segmented nanowires and colloidal nanocrystals for polarized color enrichment in displays. Here well-controlled in-template synthesis of these nanowires together with their alignment under magnetic field allows for highly parallel orientation of the nanowires in massive numbers over large-area thin films. Integrating with color-enriching nanocrystals, this enabled a record high polarization contrast over 15:1 for the isotropic nanocrystals in the visible range. We believe that such hybrid assemblies of solution-processed nanostructures integrated into optoelectronic devices hold great promise for advanced functions in photonics.

Yarıiletken nanokristallerin koloidal sentezi ve katıklanması

Colloidal semiconductor nanocrystals have drawn great interest for application areas in photonics and optoelectronics thanks to their superior optical properties including strong bandgap emission and tunability. Also, their suitability for solution-based processing has made them highly attractive for low-cost production of light-emitting diodes and lasers. Our objective in this thesis is to show the potential and versatility of semiconductor nanocrystals via colloidal synthesis and post-processing methods. The thesis work includes the synthesis of colloidal quantum dot and well structures and their post-doping and investigates their exciton decay dynamics. In this thesis a novel colloidal approach for the doping of zinc blende colloidal quantum wells was proposed and demonstrated for the first time. This new doping method uniquely relies on atomic layer deposition (ALD) process. Here we achieved the world's first manganese-doped CdSe@CdS core@shell nanoplatelets using our technique of ALD-assisted doping. Also, we studied silver-doped CdTe quantum dots under different conditions. Our experimental work proved that the quantum yield enhancement of silver-doped CdTe quantum dots is a strong function of the nanocrystal size and doping concentration. Tuning the nanocrystal size and doping level, our aqueous core-only CdTe nanocrystals reached a record high photoluminescence quantum efficiency of 68%. For these quantum dots, various decay kinetics were proposed and the enhancement in the quantum yield was attributed to the trap state annihilation. The methods and results provided in this thesis contribute to the fundamental understanding of semiconductor nanocrystals and pave the way for high-performance colloidal platforms and devices.

Çözelti halinde işlenen kuantum kuyusu yığınlarında eksiton dinamiklerinin çalışması

Yüksek verimli ışık üretimi için melez çekirdek-kabuk mimarili yenilikçi dizayn temelli kompleks nanoyapılar

Recent developments in nanoscience and nanotechnology have given rise to the discovery of hybrid nanostructured multi-component materials that serve several tasks all at once. A very important and rapidly growing field of these materials is the development of highly efficient fluorophores to meet the urgent demand of low-energy consuming, high-quality light emitters for future solid-state lighting applications. Such hybrid nanomaterials are entailed to exhibit extraordinary optoelectronic properties compared to the bulk case of their single components such as enhanced quantum efficiency, tunable multi-color emission, and reduction of multiple processing steps. Herein, to address these requirements, we propose and demonstrate novel design-based complex nanomaterials in hybrid multi-shell architectures for high-efficiency light generation. These requirements are made possible by using the concept of hybrid core-shell-? nanostructures comprising at least two units, including hybrid metal-core/dielectric-shell nanoparticles furnished with an outer shell of semiconductor nanocrystals for enhanced emission and different conjugated polymers forming a single multi-polymer nanoparticle and emitting simultaneously at different wavelengths. In the first part of this thesis, we developed and demonstrated Au-silica core/shell nanoparticles that successfully assemble CdTe nanocrystals right on their silica shells for enhanced plasmon-exciton interactions, while solving the common problems of lacking control in dielectric spacing and limited film thickness typically encountered in such plasmon-coupled nanocrystals. Here we present the synthesis and characterization results of this new set of multi-shell decorated nanoparticle composites with a tunable dielectric spacing thickness of silica shell precisely controlled by synthesis to optimize plasmon-exciton interactions for enhanced emission. Experimental data obtained from steady-state and time-resolved photoluminescence measurements together with extensive computational analysis clearly verify the strong plasmon-exciton interactions in these design-based multi-shell nanocomposites. In the second part, we construct bi-polymer nanoparticle systems in various architectures of core/shells, for each of which thorough investigations of the non-radiative energy transfer mechanisms are made. Here we present the synthesis and characterization results of these core/shell bi-polymer nanoassemblies. The flexibility of designing such bi-polymer nanostructures allows for the optimization of maximum energy transfer efficiency. This concept of complex hybrid nanostructures for high-efficiency light generation opens up new paths for optoelectronic devices and nanophotonics applications including those in solid-state lighting.

İnce-film organik güneş hücrelerinde optik soğrulmayı artırmak için tasarlanmış yeni hacimsel plazmonik rezonatör mimarileri

There has been a growing interest in decreasing the cost and/or increasing the efficiency of clean renewable energy resources including those of photovoltaic approaches for conversion of sunlight into electricity. Today, although photovoltaics is considered a potential candidate in diversification of energy sources, the cost of photovoltaic systems remains yet to be reduced by several factors to compete with fossil fuel based energy production. To this end, new generation solar cells are designed to feature very thin layers of active (absorbing) materials in the order of tens of nanometers. Though this approach may possibly decrease the cost of solar cells, these ultra-thin absorbing layers suffer from undesirably low optical absorption of incident photons. Recently revolutionary efforts on increasing light trapping using nanopatterned metal layers in the active photovoltaic material via surface plasmon excitations have been demonstrated, which attracted interest of the academic community as well as the industry. In these prior studies, plasmonic structures, placed either on the top or at the bottom of absorbing layers, have been investigated to enhance the absorption in the active material. However, all these previous efforts were based only on using a single layer of plasmonic structures. In this thesis, different than the previous reports of our group and the others, we focus on a new design concept of volumetric plasmonic resonators that relies on the idea of incorporating two (or more) layers of coupled plasmonic structures embedded in the organic solar cells. For proof-of-concept demonstration, here we embody one silver grating on the top of the absorbing layer and another at the bottom of the active layer to couple them with each other such that the resulting field localization is further increased and extended within the volume of the active material. In addition to individual plasmonic resonances of these metallic structures, this allows us to take the advantage of the vertical interaction in the volumetric resonator. Our computational results show that this architecture exhibits a substantial absorption enhancement performance particularly under the transverse-magnetic polarized illumination, while the optical absorption is maintained at a similar level as the top grating alone under the transverse-electric polarized illumination. As a result, the optical absorption in the active layer is enhanced up to ~67%, surpassing the improvement limit of individual gratings, when the total film thickness is kept fixed. This volumetric interaction contributes to further enhancement of optical absorption in the active layer, beyond the limited photon absorption in non-metallic (bare) organic solar cell.

Yarı iletken kuvantum noktacıklarında plazmon-ekziton güçlü etkileşim alanında ışınımsal olmayan enerji transfer mekanizmalarının sıralandırılması ve değiştirilmesi

Nonradiative energy transfer finds important applications in nanophotonics and nanobiotechnology including nanoscale optical waveguiding and biological nanosensors. Various fluorophores can take part in such energy transfer interactions in close proximity of each other. Their emission kinetics can be strongly modified and controlled as a result. For example, colloidal semiconductor quantum dots, also known as nanocrystals, have widely been shown to serve as donors and acceptors among themselves or with other fluorescent species to transfer excitation energy nonradiatively. In their close proximity, emission characteristics of such fluorophores can also be altered when coupled with plasmonic structures, e.g., metal nanoparticles. One favored result of these plasmon-exciton interactions is the emission enhancement. In principle it is possible to plasmon-couple acceptor-donor pairs of nonradiative energy transfer to modify their transfer rate. Such plasmon-mediated energy transfer has been demonstrated, where both acceptor-donor pairs are plasmon-coupled. In these cases, however, the resulting plasmon-exciton interactions are not controlled to take place either at the donor site or the acceptor site but at both of the sites. Therefore, it has previously not been possible to identify the coupled interactions. In this thesis, we propose and demonstrate cascaded plasmonic - nonradiative energy transfer interactions that are controlled by selectively plasmon-coupling either only the donor quantum dots or only the acceptor quantum dots. For that, we designed a novel self-assembly architecture of our hybrid layered systems of semiconductor nanocrystals and metal nanoparticles in a bottom-up fashion through precise spatial and spectral control. This scheme uniquely allowed for the ability to spatially control plasmon-exciton interactions to take place either at the ?start? site (donors) or ?finish? site (acceptors) of the energy transfer. This control was achieved by placing the plasmonic layer in the right proximity of the donors (for strong donor-exciton plasmon-coupling) while sufficiently being far away from the acceptors (for weak acceptor-exciton plasmon-coupling), or vice versa. Here we comparatively studied and analyzed consequent modifications of quantum dot emission kinetics in response to both cases of plasmon-coupling to only the donors and to only the acceptors through steady-state and time-resolved photoluminescence measurements, along with their lifetime and rate calculations. Such cascaded energy transfer interactions in the strong exciton-plasmon coupling region hold great promise for innovative near-field photonic devices and biological tags.system.

Metamalzeme özgün kablosuz RF-biyomems implant sensörler

Today approximately one out of ten patients with a major bone fracture does not heal properly because of the inability to monitor fracture healing. Standard radiography is not capable of discriminating whether bone healing is occurring normally or aberrantly. To solve this problem, we proposed and developed a new enabling technology of implantable wireless sensors that monitor mechanical strain on implanted hardware telemetrically in real time outside the body. This is intended to provide clinicians with a powerful capability to asses fracture healing following the surgical treatment. Here we present the proof-of-concept in vitro and ex vivo demonstrations of bio-compatible radio-frequency (RF) micro-electro-mechanical system (MEMS) strain sensors for wireless strain sensing to monitor healing process. The operating frequency of these sensors shifts under mechanical loading; this shift is related to the surface strain of the implantable test material. In this thesis, for the first time, we developed and demonstrated a new class of bio-implant metamaterial-based wireless strain sensors that make use of their unique structural advantages in sensing, opening up important directions for the applications of metamaterials. These custom-design metamaterials exhibit better performance in remote sensing than traditional RF structures (e.g., spiral coils). Despite their small size, these meta-sensors feature a low enough operating frequency to avoid otherwise strong background absorption of soft tissue and yet yield higher Q-factors (because of their splits with high electric field density) compared to the spiral structures. We also designed and fabricated flexible metamaterial sensors to exhibit a high level of linearity, which can also conveniently be used on non-flat surfaces. Innovating on the idea of integrating metamaterials, we proposed and implemented a novel architecture of `nested metamaterials? that incorporate multiple split ring resonators integrated into a compact nested structure to measure strain telemetrically over a thick body of soft tissue. We experimentally verified that this nested metamaterial architecture outperforms classical metamaterial structures in telemetric strain sensing. As a scientific breakthrough, by employing our nested metamaterial design, we succeeded in reducing the electrical length of the sensor chip down to ?o/400 and achieved telemetric operation across thick soft tissue with a tissue thickness up to 20 cm, while using only sub-cm implantable chip size (compatible with typical orthopaedic trauma implants and instruments). As a result, with nested metamaterials, we successfully demonstrated wireless strain sensing on sheep?s fractured metatarsal and femur using our sensors integrated on stainless steel fixation plates and on sheep?s spine using directly attached sensors in animal models. This depth of wireless sensing has proved to suffice for a vast portfolio of bone fracture (including spine) and trauma care applications in body, as also supported by ongoing in vivo experiments in live animal models in collaboration with biomechanical and medical doctors. Herein, for all generations of our RF-bioMEMS implant sensors, this dissertation presents a thorough documentation of the device conception, design, modeling, fabrication, device characterization, and system testing and analyses. This thesis work paves the way for ?smart? orthopaedic trauma implants, and enables further possible innovations for future healthcare.

Yüksek kaliteli, verimli ışık üretilmesi için ışınımsal olan ve olmayan enerji transferi kullanan, nanokristal ile tümleştirilmiş özgün LED?ler

To combat environmental issues escalating with the increasing carbon footprint, combined with the energy problem of limited resources, innovating fundamentally new ways of raising energy efficiency and level of energy utilization is essential to our energy future. Today, to this end, achieving lighting efficiency is an important key because artificial lighting consumes about 19% of total energy generation around the globe. There is a large room for improving lighting efficacy for potential carbon emission cut. However, the scientific challenge is to reach simultaneously high-quality photometric performance. To address these problems, we proposed, developed and demonstrated a new class of color-conversion light emitting diodes (LEDs) integrated with nanophosphors of colloidal quantum dots. The favorable properties of these semiconductor nanocrystal quantum dots, including size-tuneable and narrow-band emission with high photostability, have provided us with the ability of achieving high-quality, efficient lighting. Via using custom-design combinations of such nanocrystal emitters, we have shown that targeted white luminescence spectra can be generated with desired high photometric performance, which is important for obtaining application-specific white LEDs, e.g., for indoors lighting, street lighting, and LED-TV backlighting. Furthermore, dipole-dipole coupling capability of these semiconductor nanocrystals has allowed us to realize novel device designs based on Förster-type nonradiative energy transfer. By mastering exciton-exciton interactions in color-conversion LEDs, we have demonstrated enhanced color conversion via recycling of trapped excitons and white light generation based on nonradiative pumping of nanocrystal quantum dots for color conversion.This research work has led to successful demonstrators of semiconductor nanocrystal quantum dots that photometrically outperform conventional rare-earth phosphor powders in terms of color rendering, luminous efficacy of optical radiation, color temperature and scotopic/photopic ratio for the first time.Keywords: Light emitting diodes, solid state lighting, nanocrystals, quantum dots, color conversion, nonradiative energy transfer, exciton-exciton interactions.

Yenilikçi nanoparçacık içeren nanokompozit kaplamalar

Incorporating nanoparticles into nanocomposite thin-films enables coatings with multi-functionality depending on the particle type and size, and the film morphology. These multiple functions may include, for example, combinations of photocatalysis, hydrophobicity, scratch resistance, and antibacterial property. Here we proposed and demonstrated a new encapsulation nanocomposite with controllable refractive index and potentially additional functional properties for coating photonic devices, for instance, light-emitting diodes (LEDs). To design and implement this nanocomposite coating with tunable refractive index, we employed TiO2 nanoparticles of various diameters because of their relatively high refractive index. We embedded these nanoparticles in our encapsulation sol-gel material during synthesis. In addition, we incorporated several polymer-forming chemicals during synthesis to control additional functions such as hydrophobicity and scratch resistance. We used characterization tools of atomic force microscopy, refractometry, contact angle measurement, and scanning electron microscopy to study material properties.

Nanofosforların yüksek verimlilik yüksek kalite led uygulamaları için renk bilimi ve teknolojisi

Today almost one-fifth of the world?s electrical energy is consumed for artificial lighting. To revolutionize general lighting to reduce its energy consumption, high-efficiency, high-quality light-emitting diodes (LEDs) are necessary. However, to achieve the targeted energy efficiency, present technologies have important drawbacks. For example, phosphor-based LEDs suffer from the emission tail of red phosphors towards longer wavelengths. This deep-red emission decreases substantially the luminous efficiency of optical radiation. Additionally, the emission spectrum of phosphor powders cannot be controlled properly for high-quality lighting, as this requires careful spectral tuning. At this point, new nanophosphors made of colloidal quantum dots and crosslinkable conjugated polymer nanoparticles have risen among the most promising alternative color convertors because they allow for an excellent capability of spectral tuning. In this thesis, we propose and present high-efficiency, high-quality white LEDs using quantum dot nanophosphors that that exhibit luminous efficacy of optical radiation ?380 lm/Wopt, color rendering index ?90 and correlated color temperature ?4000 K. We find that Stoke?s shift causes a fundamental loss >15%, which limits the maximum feasible luminous efficiency to 326.6 lm/Welect. Considering a state-of-the-art blue LED (with 81.3% photon conversion efficiency), this corresponds to 265.5 lm/Welect. To achieve 100 and 200 lm/Welect, the layered quantum dot films are required to have respective quantum efficiencies of 39 and 79%. In addition, we report our numerical modeling and experimental demonstrations of the quantum dot integrated LEDs for the different vision regimes of human eye. Finally, we present LEDs based on the color tuning capability of conjugated polymer nanoparticles for the first time. Considering the outcomes of this thesis, we believe that our research efforts will help the development and industrialization of white light emitting diodes using nanophosphor components.

Yarı iletken nanokristal kuvantum noktacıkların ışımalı ve ışımasız enerji transferi kullanımı ile verimliliği artırılmış melez ışık yayan diyotlar ve güneş gözeleri

Today the world energy demand has overtaken unprecedented consumption levels, which have never been reached before in the history of the world. The current trends indicate that the increasing demand for energy will tend to continue at an increasing pace in the coming decades due to worldwide globalization and industrialization. Scientific community is challenged to devise and develop fundamentally new technologies to cope with the energy problem of the world. To this end, optoelectronics can offer several solutions for energy efficiency both in light harvesting and generation. In this thesis, we propose and demonstrate enhanced light generation and harvesting by utilizing both radiative and nonradiative energy transfer capabilities of semiconductor nanocrystal quantum dots, which are profited for the development of novel hybrid devices combining superior properties of the constituent material systems. One of our proposals in this thesis relies on grafting nanostructured light emitting diodes with nanocrystal quantum dots to realize highly efficient color conversion. To the best of our knowledge, we report the highest nonradiative energy transfer efficiency of 83% obtained at room temperature for this type of color-conversion light emitting diodes owing to the architectural superiorities of their nanostructure. In another proposal, we addressed charge injection problems of electrically pumped nanocrystal-based light emitting diodes. We proposed and demonstrated the utilization of novel excitonic injection scheme to drive such LEDs of nanocrystals, which may become prominent especially for the display technology. Finally, we proposed and implemented quantum dot down-conversion layers in nanostructured silicon solar cells to benefit the advantages of their nanostructured architecture. We have shown that nanostructured silicon solar cells lead to stronger enhancements compared to the planar counterparts.

Metamalzeme mimarilerinden esinlenilerek oluşturulan orijinal optik antenler

The spatial resolution of conventional optical systems is commonly constrained by the diffraction limit. This is a fundamental problem important for various high-tech applications including density limitation in data storage devices (CD, DVD, and Blue-ray discs), crosstalk in detectors, and blurred images in microscopy. To overcome this limit, different types of optical antennas have been investigated to date. However, these antennas either do not exhibit a maximum level of field intensity enhancement that can be achieved via field localization using plasmons or they have large field intensity enhancement at the cost of complicated three-dimensional architectures or very sharp tips, which are hard to fabricate. In this thesis, to address this problem, we investigate a new class of planar optical antennas inspired by metamaterial architectures including E-shape and comb shape. We found that the field intensity enhancements inside the gap regions of such comb-shaped nanoantennas were significantly increased compared to the single or array of dipoles, despite operating across an electrical length significantly reduced with respect to their resonance wavelength. We also showed that the field intensity localization of a single dipole nanoantenna can be at least doubled using single ring resonator with the same gap size by decreasing field radiations from end points and obtaining continuous current flow. These results indicate that comb-shaped planar nanoantennas hold great promise for strong field localization.

Manyetik rezonans görüntüleme için dağılımsal yüklenmiş implant edilebilir özgün esnek rezonatörler

Magnetic resonance imaging (MRI) is an enabling technology platform for imaging applications. In MRI, the imaging frequency falls within the radio frequency (RF) range where the tissue absorption of electromagnetic power is conveniently very low (e.g., compared to X-ray imaging), making MRI medically safe. As a result, MRI has evolved into a major imaging tool in medicine. However, in MRI, it is typically difficult to receive a magnetic resonance signal from tissue near a metallic implant, which hinders imaging of the implant device neighborhood to observe, monitor, and make assessment of the recovery and tissue compatibility. This can be accomplished by using locally resonating implants, but such implantable local resonators compatible with MRI that simultaneously feature reasonable chip size are currently not available (although there are some MRI-guided catheter applications). In this thesis, we proposed and developed a new class of implantable chip-scale local resonators that operate at radio frequencies of MRI, despite their small size, for the purposes of enhancing the signal-to-noise ratio (SNR) and thus the resolution in their vicinity. Here we addressed the scientific challenge of achieving low resonance frequency while maintaining chip-scale size suitable for potential MR-compatible implants. Using only biocompatible materials (gold, nitrides, and silicon or polyimide) within a substantially reduced footprint (miniaturized by 2 orders of magnitude), we demonstrated novel chip-scale designs based on the basic concept of split ring resonators (SRRs). Different than classical SRRs or those loaded with lumped elements (e.g., thin-film lumped loading), however, in our designs we loaded the SRR geometry in a distributive manner with a micro-fabricated dielectric thin-film layer to increase effective capacitance. For a proof-of-concept demonstration, we fabricated 20 mm ? 20 mm resonators that operate at the resonance frequency of 130 MHz (compatible with 3 T MRI system) when distributively loaded with the capacitive film, which would otherwise operate around 1.2 GHz as a classical SRR of the same size if not loaded. It is worth noting that this resonance frequency of 130 MHz would normally require a classical SRR of 20 cm ? 20 cm, a chip size 100-fold larger than ours. Designing and fabricating flexible thin-film resonators, we also showed that this architecture can be tuned by bending and is appropriate for non-planar surfaces, which is often the case for in vivo imaging. The phantom images indicated that, depending on the resonator configuration, these novel self-resonating structures increase SNR of the received signal by a maximum factor of 4 to 150 and over an enhancement penetration up to 10 mm into the phantom. This corresponds to a resolution enhancement in the 2D image by a factor of 2 to 12, respectively, under the same RF power. These in vitro experiments prove that it is possible to operate our local resonators at reduced frequencies via the help of distributive loading on the same chip. These findings suggest that proposed implantable resonator chips make promising candidates for self-resonating MR-compatible implants.

Nanokristalli eksiton hasati sistemleri

Semiconductor nanocrystals, also known as colloidal quantum dots, have gained substantial scientific interest for innovative light harvesting applications including those in biolabeling. Organic dyes and fluorescent proteins are widely used in biotargeting and live cell imaging, but their intrinsic optical properties, such as narrow excitation windows, limit their potential for advanced applications, e.g., spectral multiplexing. Compared to these organic fluorophores, favorable properties of the quantum dots including high photoluminescence quantum yields together with tunable emission peaks and narrow spectral emission widths, high extinction coefficients, and broad absorption bands enable us to discover and innovate light harvesting composites. In such systems, however, the scientific challenge is to achieve high levels of energy transfer from one species to the other, with additional features of versatility and tunability.To address these problems, as a conceptual advancement, this thesis proposes and demonstrates a new class of versatile light harvesting systems of semiconductor nanocrystals mediated by excitonic interactions based on Förster-type nonradiative energy transfer. In this thesis, we synthesized near-unity efficiency colloidal quantum dots with as-synthesized photoluminescence quantum yields of >95%. As proof-of-concept demonstrations, we studied and achieved highly efficient exciton harvesting systems of quantum dots bound to fluorescent proteins, where the excitons are zipped from the dots to the proteins in the composite. This led to many folds of light harvesting (tunable up to 15 times) in the case of the green fluorescent protein. Using organic dye molecules electrostatically interacting with quantum dots, we showed high levels of exciton migration from the dots to the molecules (up to 94%). Furthermore, we demonstrated stand-alone, flexible membranes of nanocrystals in unprecedentedly large areas (> 50 cm × 50 cm), which paves the way for high-end, large-scale applications. In the thesis, we also developed exciton-exciton coupling models to support the experimental results. This thesis opens up new possibilities for exciton-harvesting in biolabeling and optoelectronics.Keywords: Semiconductor nanocrystals, nonradiative energy transfer, excitons, light harvesting.

Çevre dostu ınp/zns nanokristaller

Semiconductor nanocrystals are nanometer scale fluorescent crystallites with tunable optical properties, which can be controlled by the material composition and particle size. They can be prepared using various synthesis techniques and find applications in many different areas ranging from life sciences to electronics. In this thesis, indium phosphide based nanocrystals are studied for LED applications. The thesis research work focuses on the colloidal synthesis method and material characterization of these nanocrystals. Using one pot synthesis method, the indium phosphide/zinc sulfide (InP/ZnS) core/shell nanocrystal structures are synthesized. This synthesis technique allows for a reproducible and tunable preparation method. The material characterization techniques used in this thesis include UV-Vis spectroscopy, photoluminescence spectroscopy, transmission electron microscopy (TEM), X-ray diffraction, X-ray photoelectron spectroscopy (XPS), inductively coupled plasma-mass spectrometry (ICP-MS), and Zeta Sizer (or DLS). These properties make InP/ZnS nanocrystals comparable to their cadmium (Cd) containing counterparts with respect to their optical properties, and InP/ZnS nanocrystals offer the potential to replace them because of environmental concerns in LED applications.

Küresel kuantum noktalarının optik yakın alan etkileşimi

Nanometer-sized materials can be used to make advanced photonic devices. However, as far as the conventional far-field light is concerned, the size of these photonic devices cannot be reduced beyond the diffraction limit of light, unless emerging optical near-fields (ONF) are utilized. ONF is the localized field on the surface of nanometric particles, manifesting itself in the form of dressed photons as a result of light-matter interaction, which are bound to the material and not massless. In this thesis, we theoretically study a system composed of different-sized quantum dots involving ONF interactions to enable optical excitation transfer. Here this is explained by resonance energy transfer via an optical near-field interaction between the lowest state of the small quantum dot and the first dipole-forbidden excited state of the large quantum dot via the dressed photon exchange for a specific ratio of quantum dot size. By using the projection operator method, we derived the formalism for the transfered energy from one state to another for strong confinement regime for the first time. We performed numerical analyses of the optical near-field energy transfer rate for spherical colloidal quantum dots made of CdSe, CdTe, CdSe/ZnS and PbSe. We estimated that the energy transfer time to the dipole forbidden states of quantum dot is sufficiently shorter than the radiative lifetime of excitons in each quantum dot. This model of ONF is essential to understanding and designing systems of such quantum dots for use in near-field photonic devices.

SILAR tekniği ile çok verimli CdSe/CdS çekirdek/kabuk nanokristal kuvantum noktacıklarının sentezi ve karakterizasyonu

Owing to their size tunable electronic structure and optical properties, semiconductor nanocrystal quantum dots (NQDs) have become attractive for a wide range of device applications ranging from life sciences to electronics in the last two decades. However, highly efficient and stable NQDs are essential to reaching high performance with these devices utilizing NQDs. In this thesis, to meet these requirements, a new class of CdSe/CdS core/shell NQDs are studied including their colloidal synthesis and nanocharacterization. In this work, CdSe/CdS core/shell NQDs were synthesized with successive ion layer adsorption and reaction (SILAR) technique, which enabled highly precise shell thickness control and uniform coating of the shell material.When compared to the most commonly used CdSe/ZnS core/shell NQDs, CdSe/CdS core/shell NQDs were found to provide important advantages. First, the lattice mismatch within CdSe and CdS (3.9%) is lower than that within CdSe and ZnS (12%), which was very critical for obtaining highly efficient NQDs. Second, as a result of having lower bandgap in CdS, great enhancement in absorption cross section was achieved with more red-shifted emission, which is not possible with CdSe/ZnS core/shell NQDs. Moreover, suppression of Auger recombination was successfully observed with the partial separation of electron and hole wavefunctions in the synthesized CdSe/CdS core/shell NQDs. With all these attractive properties that were experimentally measured, CdSe/CdS core/shell NQDs were found to make better alternatives to CdSe/ZnS core/shell for numerous applications.Keywords: semiconductor nanocrystals, nanocrystal quantum dots, colloidal synthesis.

InGaN/GaN kuvantum yapılarının ve aygıtlarının elektrik alana bağlı optoelektronik doğası

In the past two decades we have been witnessing the emergence and rapid development of III-Nitride based optoelectronic devices including InGaN/GaN light-emitting diodes (LEDs) and laser diodes with operation wavelengths ranging from green-blue to near-UV. These InGaN/GaN devices are now being widely used in applications important for lighting, displays, and data storage, collectively exceeding a total market size of 10 billion USD. Although InGaN/GaN has been studied and exploited very extensively to date, its field dependent nature is mostly unknown and is surprisingly prone to quite unexpected behavior due to its intrinsic polarization property. In this thesis, we report our systematic study on the electric field dependent characteristics of InGaN/GaN quantum structures and devices including modulators and LEDs. Here we present our comparative study of electroabsorption in polar c-plane InGaN/GaN multiple quantum wells (MQWs) with different built-in polarization induced electrostatic fields. Analyzing modulator structures with varying structural MQW parameters, we find that electroabsorption grows stronger with decreasing built-in electrostatic field strength inside the well layer, as predicted by our theoretical model and verified by our experimental results. To further explore the field dependent optoelectronic nature of c-plane grown InGaN/GaN quantum structures, we investigate radiative carrier dynamics, which is of critical importance for LEDs. Our time and spectrum resolved photoluminescence measurements and numerical analyses indicate that the carrier lifetimes, the radiative recombination lifetimes, and the quantum efficiencies all decrease with increasing field. We also study the physics of electroabsorption and carrier dynamics in InGaN/GaN quantum heterostructures grown intentionally on nonpolar a-plane of the wurtzite crystal structure, which are free of the polarization-induced electrostatic fields. We compare these results with the conventional c-plane grown polar structures. In the polar case, we observe blue-shifting absorption profile and decreasing carrier lifetimes with increasing electric field. In the nonpolar case, however, we observe completely the opposite: a red-shifting absorption profile and increasing carrier lifetimes. We explain these observations in the context of basic physical principles including Fermi?s golden rule and quantum-confined Stark effect. Also, we present electroabsorption behavior of InGaN/GaN quantum structures grown using epitaxial lateral overgrowth (ELOG) in correlation with their dislocation density levels and in comparison to steady state and time-resolved photoluminescence measurements. The results reveal that ELOG structures with decreasing mask stripe widths exhibit stronger electroabsorption performance. While keeping the ELOG window widths constant, compared to photoluminescence behavior, however, electroabsorption surprisingly exhibits the largest performance variation, making the electroabsorption the most sensitive to the mask stripe widths. This thesis work provides significant insight and important information for the optoelectronics of InGaN/GaN quantum structures and devices to better understand their field dependent nature.

Üç boyutlu plazmonik yüzezler: Modelleme, nanofabrikasyon ve karakterizasyon

-Today designing functional nanoplasmonic structures specific to a variety of applications attracts great interest from various fields ranging from optoelectronics to life sciences. There are numerous ways of making nanoplasmonic structures. Among them, nanopatterning of a thin-film metal layer is one of the most common approaches, which allows for finely controlled fabrication of a plasmonic unit and their repeating layout in the plane of the starting metal film. Although there are many examples of such nanopatterned plasmonic structures reported to date, they are typically designed and implemented on a planar surface. In these architectures, plasmonic layout commonly covers significantly less than 100% of the substrate surface and can provide field localization most strongly around the sharp corners and small gaps between the patterns. In the case of using a periodic layout, which is commonly employed for experimental realization (although periodicity is not necessary), the plasmonic array inherently yields a duty cycle substantially less than unity (usually close to 0.5). As a result, the surface coverage of nanopatterned plasmonic structures on a planar surface has intrinsically been limited and the field enhancement across their nanoplasmonic layout has been possible mostly in the plane and slightly above it. To address these limitations, this thesis proposed and demonstrated three-dimensional (3D) nanoplasmonic arrayed structures designed and implemented on a non-planar surface that allows for strong field enhancement in the out-of-plane direction and enables a very large surface coverage of the substrate close to unity. The thesis work included both ivnumerical modeling and experimental characterizations. As a proof-of-concept demonstration, we fabricated non-planar arrays of checkerboard nanostructures, each with two-fold rotational symmetry, laid out in a volumetric fashion as two interlocked square lattice arrays at two different levels, facilitating strong field localization vertically between these two complementary planes. The resulting nanofabricated samples exhibited a maximum surface coverage of 100% in planview. With full electromagnetic solution of such 3D nanoplasmonic surfaces, we showed that the out-of-plane field localization is 7.2-fold stronger than the inplane localization, in comparison to their two-dimensional (2D) components alone. These numerical results agree well with the experimental observations including far-field optical transmission and reflection measurements. The absorption spectroscopy further revealed that the resulting spectrum of the 3D checkerboard features a unique signature arising from the out-of-plane localization, which does not exist in the case of the 2D counterparts. These results indicate that 3D nanoplasmonics of such non-planar surfaces provides us with the ability to generate and better utilize the plasmonic volume, possibly useful for increased plasmonic coupling and interactions.Keywords: Plasmonics, plasmonic nanostructures, FDTD simulation, nanofabrication

Yarı iletken nanokristallerde çoklu eksiton oluşturması ve yeniden birleşimi: Temel bilimsel anlama ve uygulamalar

Semiconductor nanocrystal quantum dots (QDs) have been found to be very promising for important application areas in optoelectronics and photonics. Their energy band-gap tunability, high performance band-edge emission, decent temperature stabilities, and easy material processing make the QDs attractive for these applications ranging from photovoltaic devices to photodetectors and lasers to light-emitting diodes. For these QDs, the concepts of multi exciton generation (MEG) and recombination (MER) have recently been shown to be important especially because they possibly enable efficiency levels exceeding unity using these QDs in various device configurations. However, understanding multi exciton kinetics in QD solids has been hindered by the confusion of MER with the recombination of carriers in charged QDs. This understanding lacks to date and the spectral-temporal aspects of MER still remain unresolved in solid QD ensembles. In this thesis, we reveal the spectral-temporal behavior of biexcitons (BXs) in the presence of photocharging using near-unity quantum yield core/shell CdSe/CdS QDs. The spectral behavior of BXs and that of excitons (Xs) were obtained for the QD samples with different core sizes, exhibiting the strength-tunability of the X-X interaction energy in these QDs. The extraction of spectrally resolved X, BX, and trion kinetics, which would be spectrally unresolved using conventional approaches, is enabled by our approach introducing the integrated time-resolved fluorescence. Besides the fundamental understanding of MEG and MER concepts, we also explored the possibility of utilizing multi excitons in these QDs for optical gain. In this part of the thesis, tunable, high performance, two-photon absorption (TPA) based amplified spontaneous emission (ASE) from the same QDs is presented. Here, for the first time, in addition to the absolute spectral tuning of the ASE, on the single material system of CdSe/CdS, the relative spectral tuning of ASE peak with respect to spontaneous emission was demonstrated. With the core and shell size adjustments, it was shown that Coulombic X-X interactions can be tuned to be either attractive leading to the red-shifted ASE peak or repulsive leading to the blue-shifted ASE peak and that non-shifting ASE can be achieved with the right core-shell combinations. It was further found here that it is possible to obtain ASE at a specific wavelength from both Type-I-like and Type-II-like CdSe/CdS QDs. In addition to the CdSe/CdS QDs, we showed ASE and Type-tunability features on CdSe/CdS nanorods (NRs), which are particularly promising with their extremely high TPA cross-sections and independent emission/absorption tunabilities. In the final part of the thesis, we report the observation of MEG on CdHgTe QDs, for the first time in the literature, and a novel application of MEG concept in a photosensor device, one of the first examples of real-life photosensing application of MEG concept. We believe that the results provided in this thesis do not only contribute to the fundamental understanding of MEG and MER concepts in the QDs, but also pave the way for the utilization of these concepts in the QD-based lasers, photodetectors and photovoltaic devices.

Yarı iletken tip I ve tip II çekırdek/kabuk nanokristallerdeki eksiton ve bieksitonların hesaplamalı incelemesi

In this thesis, we studied electronic structure and optical properties of Type-I, Type-II, and quasi Type-II semiconductor nanocrystals (also known as colloidal quantum dots). For a parametric study, we developed quantum mechanical models and solved them using both analytical and numerical techniques. The simulation results were compared to the experimental findings. We showed that charge carrier localization at different spatial locations could be tuned by controlling size parameters of the core and shell. While tuning charge localization, we also predicted photoluminescence peaks of these core/shell nanocrystals using our theoretical and numerical calculations. We demonstrated that Type-II nanocrystals exhibit different tuning trends compared to the Type-I ones. We also investigated biexcitonic properties of nanocrystals using quantum mechanical simulations, which are important especially in lasing applications. We showed that two-photon absorption mechanism can be tuned by changing the core and shell size in quantum dots. We calculated at which core and shell sizes biexcitons in quantum dots show attractive or repulsive interaction. The computational studies presented in this thesis played an important role in the experimental demonstrations and understanding of controlling excitonic features of core/shell nanocrystals.

Nanokristal tabanlı ışığa duyarlı yenilikçi yüzeyler

Light sensing devices traditionally made from crystalline or amorphous silicon, operating at the visible and near-infrared wavelengths, have led to a multibillion-dollar annual market. However, silicon faces various limitations including weak detection at long wavelengths (insufficient beyond 1.1 µm) with a cut-off at short wavelengths (in the ultraviolet) and small-area applications. On the other hand, solution-processed semiconductor nanocrystals (NCs), also known as colloidal quantum dots, offer large-area light sensing platforms with strong absorption cross-section. In this thesis we propose and demonstrate a new class of large-area, semi-transparent, light-sensitive nanocrystal skin (LS-NS) devices intended for large-surface applications including smart transparent windows and light-sensitive glass facades of smart buildings. These LS-NS platforms, which are fabricated over areas up to many tens of cm2 using spray-coating and several cm-squares using dip-coating, are operated on the basis of photogenerated potential buildup, as opposed to conventional charge collection. The close interaction of the monolayer NCs of the LS-NS with the top interfacing metal contact results in highly sensitive photodetection in the absence of external bias, while the bottom side is isolated using a high dielectric spacing layer. In operation, electron-hole pairs created in the NCs of the LS-NS are disassociated and separated at the NC monolayer - metal interface due to the difference in the workfunctions. As a result, the proposed LS-NS platforms perform as highly sensitive photosensors, despite using a single NC monolayer, which makes the device semi-transparent and reduces the noise generation. Furthermore, because of the band gap tunability, it is possible to construct cascaded NC layers with a designed band gap gradient where the NC diameters monotonically change. Here we present the first account of exciton funneling in an active device, which leads to significant performance improvement in the device. We show highly photosensitive NC skins employing the exciton funneling across the multiple layers of NC film. To further enhance the device photosensitivity performance, we demonstrate embedding plasmonic nanoparticles into the light-sensitive skins of the NCs. In addition, we exhibit the LS-NS device sensitivity enhancement utilizing the device architecture of semi-transparent tandem skins, the addition of TiO2 layer for increased charge carrier dissociation, and the phenomenon of multiexciton generation in infrared NCs. With fully sealed NC monolayers, LS-NS is found to be highly stable under ambient conditions, promising for low-cost large-area UV/visible sensing in windows and facades of smart buildings. We believe the findings presented in this thesis have significant implications for the future design of photosensing platforms and for moving toward next generation large-surface light-sensing platforms.

Kuvantum noktacıkları gömülü makrokristallerde ekziton transferi

For nonradiative energy transfer (NRET) in the field of medicine and biology as well as optoelectronics, recent advances in the fluorophores, and optical techniques and devices have led to greatly increased interest in applications employing NRET in the past decade. Replacing traditional fluorophores, colloidal quantum dots have flourished the fluorescence properties of NRET-based applications. This has also given rise to working with narrower tunable emission at a higher quantum yield with broadband absorption, and easier handling and fabrication compared to those of traditional fluorophores. A newly discovered technique, QD incorporation into macrocrystals of various salts, has enhanced the processability, photostability and robustness of these colloidal QDs. To benefit from these enhanced properties for NRET, this thesis proposed and studied macrocrystals for exciton transfer via NRET and fabricated those considering NRET mechanism. The design of these QD-embedded macrocrystal structures has enabled strong energy transfer. The experimentally measured energy transfer reached ~51%, which was obtained with careful optimization. Moreover, these hybrid structures have allowed for the observation of the QD distribution dependence of the transfer efficiency for the QDs wrapped inside macrocrystals. The steady state and time-resolved measurements in this thesis revealed that QD-incorporated macrocrystals can possibly take place of QDs in various NRET-related applications.