Phd Degree / Doktora
Permanent URI for this collectionhttps://hdl.handle.net/11147/2869
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Doctoral Thesis Development of Novel Anticounterfeiting Technologies Using Heavy Metal Free Nanoparticles(Izmir Institute of Technology, 2021) Taşcıoğlu, Didem; Özçelik, Serdar; Demir, Mustafa MuammerCounterfeiting, the act of illegally copying a product, document or currency, is a growing problem and causes economic losses. Anticounterfeiting technology uses fluorescent inks that are invisible to the naked eye in daylight, but become visible under UV light. However, these inks have problems such as fading when exposed to sunlight or room light for a long time and disappear completely over time. This is due to the relevant inks are made using organic dyes that fade. The inks used in anticounterfeiting application preventing copying of secure documents such as banknotes, passports and ID cards must be health-friendly and chemically and optically stable for years. All of the existing security materials and equipments for ID cards, driver's licenses, passports, banknotes used in our country are imported. In this study, our aim is to create a new generation of security materials and codes to combat counterfeiters and to verify the generated security codes in a simple, efficient and fast way. In this study, it is aimed to produce nanoparticles, which do not contain heavy metals and show optical stability for a long time, emitting in visible region, on the basis of the security codes created. For this purpose, water and solvent-based nanoparticles synthesized which are non-toxic should have a long-term optical stability. The synthesized nanoparticles act like a pigment in security codes. The photoluminescence (emission color) of the security codes can be adjusted by size and chemical composition of nanoparticles. In this study, colloidally monodispersed and highly photoluminescent InP based nanoparticles were synthesized by the hot-injection approach under an inert atmosphere. In addition, a protective shell (ZnS, ZnSe) coating methods have been applied to provide optical stability to InP nanoparticles. Moreover, carbon-based nanoparticles with high optical stability and being dispersible in water were synthesized using the bottom-up method. Security codes that cannot be detected in daylight have been created on different subtrates (paper, polymer, glass, etc.) by using screen printing and inkjet printing methods, which are well known printing methods using the synthesized nanoparticles. In addition, the authenticity of the security codes was checked using a commercial fiber optic based spectrometer (Ocean Optics spectrometer) and a handy hand-held optical device called the Quantag sensor developed by Quantag Nanotechnologies. Thus, a verification method that can be distinguished by a simple detection device is proposed. The synthesized nanoparticles were furthermore dispersed in a polymer solution to create random droplet and droplet/fiber patterns by electrospinning method. Thus, unique and inimitable security codes detectable under UV light were created which may be used in the fight against counterfeiting. To check the authenticity of the original security codes created; images collected with a simple smartphone microscope and a database was created in which the original patterns were recorded. The originality of the random patterns obtained was checked by comparing it with the patterns recorded in the database. In addition, the spectral information of the particle from the droplet/fiber pattern obtained was determined with a simple hand-held device (Ocean Optics optical spectrometer). Thus, by reading spectral information from the pattern, the spectral signature of the nanoparticles was determined and thus a second-step security was created. In this way, a two-stage anticounterfeiting technology that is impossible to imitate has been developed. As a conclusion, it is believed that the security codes developed in this study will pave the way for the commercialization of quantum labeling technology.Doctoral Thesis The Fabrication of Plasmonic/Photonic Nanostructures in Polymers: Mechanical Sensor Applications(Izmir Institute of Technology, 2019) Topçu, Gökhan; Demir, Mustafa Muammer; Eanes, MehtapFunctional polymer nanocomposites offer futuristic properties by the association of inorganic additive micro-/nanostructures into the polymers. With the growing knowledge of the physical fundamentals, stimuli-responsive polymeric composites enable detection of chemical, thermal, and mechanical changes by optical sensors and probes. Since the accurate real-time detection of the change in mechanical loading is vital for construction and industrial fields, the use of colorimetric pressure elements in a static body is important for the prediction of catastrophic failures. In this thesis, strain/pressure responsive colorimetric films were produced. A number of polymer nanocomposite-based mechanical sensors are presented. By transferring the optical activity (coherent reflection and plasmonic coupling) of the additives into various polymeric matrices having different mechanical features, the strain and pressure sensors are developed for practical applications. There are two approaches used for the fabrication of polymeric mechanical sensors: i) PDMS/SiO2 composites, ii) PAAm/Au NP composites. The coherent reflectivity of SiO2 colloidal particle arrays was used to develop strain sensors while controllable localized surface plasmon resonance of Au NPs was employed for pressure sensors. These optical systems were separately associated with viscoelastic and elastic polymeric systems, and sensor properties were discussed.Doctoral Thesis Development of Colloidal Alloyed Nanocrystals for Quantum Dot Based Device Applications(Izmir Institute of Technology, 2018) Sevim Ünlütürk, Seçil; Özçelik, Serdar; Varlıklı, CananQuantum dots (QDs) are very attractive luminescent semiconducting nanoparticles. In this study, our aim was to synthesize Cd and/or Zn based QDs with tunable optical properties by the particle size and the alloy composition. Colloidal water dispersible Mn-doped and nondoped ZnSxSe1-x QDs were synthesized by the one-pot aqueous method. Optical measurements indicate that photoluminescent properties are strongly depended on the capping agent. While MPA capped QDs showed an emission peak in the blue region, others did not show any photoluminescence at all. Mn doping up to 10% resulted in no significant effect on the optical spectra. However structural characterizations, EPR and XRD, supported that Mn ions were bounded to the 220 and 311 facets of QD. ZnxCd1-xSySe1-y quaternary nanoalloys were synthesized by using a modified two-phase approach for the first time in the literature. Optical properties of highly luminescent ZnxCd1-xSySe1-y nanoalloys were tuned from blue to yellow by the particle size, the alloy composition, and thickness of shell layer. The reactivity of the reactants, initial mole ratios, and other reaction parameters was adjusted to control alloy composition and alloy type: homogeneous and gradient. The reaction time controls the size of particles. The PL QE (up to 52%) and lifetimes (about 25 ns) were found similar regardless of core and core-shell nanoalloys. MicroPL measurements were carried out on ZnxCd1-xSySe1-y nanoalloys by fiber spectrometer integrated to confocal microscope. Photobleaching and blue-shifting, about 6 nm, were observed in the microPL spectra. Photobleaching times and rate constants obtained from single exponential decay curves showed that purification and exposure time are strongly effective. Additionally, the power the excitation light is essential that below 11 μW, photobleaching slows down, and at 2 μW there is no photobleaching. Scale-up methods with high-volume batch and flow reactor were used to synthesize CdTe and ZnxCd1-xSySe1-y QDs. LEFETs were fabricated with TUBITAK support in collaboration with Heidelberg University. PbS QDs were used as emitting material at the bottom contact top-gate unipolar LEFETs in which uniform electroluminescence was obtained.Doctoral Thesis Synthesis, Physicochemical Characterization, and Biosensing Applications of Gold Nanoparticles(Izmir Institute of Technology, 2018) Üçüncü, Melek; Özçelik, SerdarCancer is one of the leading diseases that cause death all around the world. In Turkey, lung cancer is the most common type of cancer type in men and it is the fifth in women. Unfortunately, the percentage of treatment of lung cancer is too low. Gold nanoparticles (AuNPs) are widely used in the biotechnology as imaging, diagnosis, and therapeutic agents because of their unique properties such as plasmon resonance, easy synthesize, biocompatibility, and facile surface modification. In this study, it is aimed to design gold nanoparticles as biosensors for lung cancer cells. For this purpose, different sizes (5-40 nm) of Au nanoparticles were synthesized and their uptake and distribution into the lung cancer cells were investigated. The results of the study revealed that cellular uptake of gold nanoparticles are high for the size of 20 and 40 nm. The optimal visibility into the cells was achieved by using DIC microscopy in which the particles uptaken into the cytoplasm and localized at around nucleus of cells. In the second part of the study, surfaces of 20 and 40 nm particles were conjugated with RGD peptides and their distribution and light scattering properties were investigated in living cells by using dark-field microscopy. Due to the receptor-mediated endocytosis, RGD-AuNPs showed different distribution within the cells. These results indicate that the RGD conjugated Au nanoparticles exhibits much higher light scattering properties than non-conjugated nanoparticles. In addition to this, synthesized Au nanoparticles were conjugated with nucleus-localized peptide (NLS) and directed to the nucleus of cancerous (A549, H358) and healthy (BEAS2B) lung cells. The nucleus targeting properties of the NLS conjugated particles were also investigated to understand if there is any cell line selectivity. The internalizations of peptide conjugated Au nanoparticles into cell lines were visualized in living cells by using DIC microscopy. NLS conjugated AuNPs internalized into nucleus of A549 and H358 cancer cells. Although NLS conjugated AuNPs present inside the cytoplasm of BEAS2B cells, they did not localize into the nucleus of normal cell lines.Doctoral Thesis Preparation and Characterization of Nanoparticles as Carriers for Gene Delivery(Izmir Institute of Technology, 2014) Uz, Metin; Altınkaya, SacideIn the first part of this thesis, a comprehensive characterization of polyethylene glycol (PEG) modified AuNPs designed for imaging or diagnostic purposed was carried out to investigate the effect of the size, PEG layer conformation and grafting density on the cellular uptake, toxicity and cell cycle phases against prostate (PC3), colon (CaCo2) cancer cell lines and 3T3 Swiss fibroblast cells. It was noticed that the cellular uptake and toxicity profiles of the particles varied depending on the size, surface properties and cell type. The particles were found to show alterations in cell cycle phases by causing DNA damage without apoptotic behavior at certain doses. In the second part of this thesis, efficient multilayer small interfering RNA (siRNA) delivery systems based on gold nanoparticles (AuNPs), cationic pentablock copolymers or fusogenic peptides were developed using cleavable disulfide bonds and electrostatic interactions. siRNA/Polymer (polyplexes) and siRNA/Peptide (peptideplexes) complexes formed by direct electrostatic complexation between siRNA and the cationic pentablock copolymers or peptides were used as controls, respectively. In addition, a conjugate siRNA delivery system based on the cleavable disulfide bonds between siRNA and fusogenic peptide was also proposed as an alternative system. The siRNA activity, toxicity, cellular uptake and intracellular distribution of the developed systems were investigated against luciferase-expressing SKOV3 ovarian cancer cell line. The use of cationic block copolymers or fusogenic peptides in AuNP based multilayer systems and complex systems, provided efficient siRNA condensation and protection from nuclease enzyme and serum protein degradation, in addition to cellular uptake, endosomal escape and siRNA activity in the cytoplasm.Doctoral Thesis Synthesis and Control of Exciton Dynamics in Cdte, Cdte/Cds and Znxcd1-Xte Colloidal Nanocrystals(İzmir Institute of Technology, 2012) Eral Doğan, Leyla; Özçelik, SerdarThe aim of this study is to synthesize cadmium-based semiconductor colloidal nanocrystals and to control their exciton dynamics by tuning the size and composition of the nanocrystals (NCs). CdTe, CdTe/CdS binary, and ZnxCd1-xTe ternary semiconductor NCs are prepared by wet chemistry. The reactions are thoroughly optimized to enhance the optical properties. The optical properties of CdTe and CdTe/CdS are tuned by the size of the NCs by adjusting the reaction (the growth) time. Coating CdTe NCs with CdS layer enhances the photoluminescence quantum yields up to 45%. ZnxCd1-xTe ternary nanoalloys were synthesized by varying the initial mole ratios of metals (Zn/Zn+Cd) and the growth time. The size and the composition-tunable ZnxCd1-xTe nanoalloys exhibit highly luminescent optical properties. When the amount of initial Zn precursor is low, the nanoalloys have Cd-rich and Zn-poor internal crystal structure. However, at higher amount of Zn precursor, the nanoalloys have Zn-rich and Cd-poor core exhibiting gradient composition. The exciton interactions and dynamics are investigated as a function of the size of CdTe/CdS, and the composition and the size of ZnxCd1-xTe nanoalloys. The exciton interaction yields amplification in the output signal at the threshold of 1015 photon/cm2s per laser pulse. The exciton lifetimes are in the range of picoseconds to nanoseconds. The decay associated spectra are affected by the laser power, size and composition of the NCs. As the laser power increases new excitonic states are created especially in ZnxCd1-xTe nanoalloys. Multiexcitons were created in the NCs depending on the laser power. Small NCs exhibit stronger exciton-exciton interactions under high laser power compared to larger NCs. However larger NCs have lesser exciton density, therefore reducing the exciton-exciton interactions.