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(1 - 14 of 14)
- Title
- SURFACE PLASMON HOSTS FOR INFRARED WAVEGUIDES AND BIOSENSORS, AND PLASMONS IN GOLD-BLACK NANO-STRUCTURED FILMS.
- Creator
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Cleary, Justin, Peale, Robert, University of Central Florida
- Abstract / Description
-
Applications of surface plasmon polaritons (SPPs) have thus far emphasized visible and near-infrared wavelengths. Extension into the long-wave infrared (LWIR) has numerous potential advantages for biosensors and waveguides, which are explored in this work. A surface plasmon resonance (SPR) biosensor that operates deep into the infrared (3-11 µm wavelengths) is potentially capable of biomolecule recognition based on both selective binding and characteristic...
Show moreApplications of surface plasmon polaritons (SPPs) have thus far emphasized visible and near-infrared wavelengths. Extension into the long-wave infrared (LWIR) has numerous potential advantages for biosensors and waveguides, which are explored in this work. A surface plasmon resonance (SPR) biosensor that operates deep into the infrared (3-11 µm wavelengths) is potentially capable of biomolecule recognition based on both selective binding and characteristic vibrational modes. The goal is to operate such sensors at wavelengths where biological analytes are strongly differentiated by their IR absorption spectra and where the refractive index is increased by dispersion, which will provide enhanced selectivity and sensitivity. Potentially useful IR surface plasmon resonances are investigated on lamellar gratings formed from various materials with plasma frequencies in the IR wavelength range including doped semiconductors, semimetals, and conducting polymers. One outcome of this work has been the demonstration of a simple analytic formula for calculating the SPP absorption resonances in the angular reflectance spectra of gratings. It is demonstrated for Ag lamellar gratings in the 6-11 µm wavelength range. The recipe is semi-empirical, requiring knowledge of a surface-impedance modulation amplitude, which is found here by comparison to experiment as a function of the grating groove depth and the wavelength. The optimum groove depth for photon-to-SPP energy conversion was found by experiment and calculation to be ~10-15% of the wavelength. Hemicylindrical prism couplers formed from Si or Ge were investigated as IR surface plasmon couplers for the biosensor application. Strong Fabry-Perot oscillations in the angular reflectance spectra for these high index materials suggest that grating couplers will be more effective for this application in the LWIR. A variety of materials having IR plasma frequencies were investigated due to the tighter SPP mode confinement anticipated in the IR than for traditional noble metals. First doped-Si and metal silicides (Ni, Pd, Pt and Ti) were investigated due to their inherent CMOS compatibility. Rutherford backscattering spectroscopy, x-ray diffraction, scanning electron microscopy, secondary ion mass spectrometry and four point probe measurements complemented the optical characterization by ellipsometry. Calculation of propagation length and mode confinement from measured permittivities demonstrated the suitability for these materials for LWIR SPP applications. Semimetals were also investigated since their plasma frequencies are intermediate between those of doped silicon and metal silicides. The semimetal antimony, with a plasma frequency ~80 times less than that of gold was characterized. Relevant IR surface plasmon properties, including the propagation length and penetration depths for SPP fields, were determined from optical constants measured in the LWIR. Distinct resonances due to SPP generation were observed in angular reflection spectra of Sb lamellar gratings in the wavelength range of 6 to 11 µm. Though the real part of the permittivity is positive in this range, which violates the usual condition for the existence of bound SPP modes, calculations based on experimental permittivity showed that there is little to distinguish bound from unbound SPP modes for this material. The SPP mode decays exponentially away from the surface on both sides of the permittivity sign change. Water is found to broaden the IR plasmon resonances significantly at 9.25 micron wavelength where aqueous extinction is large. Much sharper resonances for water based IR SPR biosensor can be achieved in the 3.5 to 5.5 µm range. Nano-structured Au films (Au-black) were investigated as IR absorbers and possible solar cell enhancers based on surface plasmon resonance. The characteristic length scales of the structured films vary considerably as a function of deposition parameters, but the absorbance is found to be only weakly correlated with these distributions. Structured Au-black with a broad range of cluster length scales appear to be able to support multiple SPP modes with incident light coupling to the corrugated surface as seen by photoelectron emission microscopy (PEEM) and SPR experiments, supporting the hypothesis that Au-black may be a suitable material for plasmon-resonance enhancement solar-cell efficiency over the broad solar spectrum.
Show less - Date Issued
- 2010
- Identifier
- CFE0003231, ucf:48547
- Format
- Document (PDF)
- PURL
- http://purl.flvc.org/ucf/fd/CFE0003231
- Title
- Development of enzyme-free hydrogen peroxide biosensor using cerium oxide and mechanistic study using in-situ spectro-electrochemistry.
- Creator
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Saraf, Shashank, Seal, Sudipta, Cho, Hyoung Jin, Zhai, Lei, Heinrich, Helge, Harper, James, University of Central Florida
- Abstract / Description
-
During recent development, it has been demonstrated that cerium oxide nanoparticles (CNPs) have exhibited catalytic activity which mimics naturally existing enzymes such as superoxide dismutase (SOD) and catalase. The underlying mechanism is attributed to the modulation of oxygen vacancies on CNPs lattice by dynamic switching of the oxidation states between Ce3+ and Ce4+ due to the electron transfer resulting from the redox reaction between CNPs and reactive oxygen species such as hydrogen...
Show moreDuring recent development, it has been demonstrated that cerium oxide nanoparticles (CNPs) have exhibited catalytic activity which mimics naturally existing enzymes such as superoxide dismutase (SOD) and catalase. The underlying mechanism is attributed to the modulation of oxygen vacancies on CNPs lattice by dynamic switching of the oxidation states between Ce3+ and Ce4+ due to the electron transfer resulting from the redox reaction between CNPs and reactive oxygen species such as hydrogen peroxide (H2O2). Thereby the redox potential of CNPs is dependent on the surface chemistry i.e. the surface concentration of Ce3+ and Ce4+ Currently, the ratio of Ce3+/ Ce4+ in CNPs is characterized ex-situ using XPS or TEM which involves sample drying and exposure to high energy X-rays and electron beam, respectively. Sample drying and high energy beam exposure could lead to sample deterioration. The goal of the study is to explore a technique to characterize CNPs in-situ and identify the surface chemistry of CNPs. The in-situ investigation of CNPs was carried using spectroelectrochemistry wherein the electrochemical and optical measurements are carried out simultaneously. Detailed optical characterization of two different CNPs having different catalytic activity were carried under oxidation and reduction environments. Analysis of spectra revealed widely different redox potential for CNPs which was a function of pH and composition of buffer solution. In second part of dissertation a suitable surface chemistry of CNPs is investigated to replace the enzyme in biosensor assembly to allow amperometric detection of H2O2 in physiological conditions. Upon electrochemical investigation of the physio-chemical properties of CNPs, it was found that CNPs having higher surface concentration of Ce4+ as compared to Ce3+ oxidation states, demonstrated increased catalytic activity towards H2O2. The addition of CNPs resulted in 5 orders of increment in amperometric current with a response time of 400 msec towards detection of H2O2 and exhibited excellent selectivity in presence of interfering species. Additionally, cerium oxide was successfully integrated into the biosensor assembly through the anodic electrodeposition, which allowed the transfer of electron generated from the CNPs in the redox reaction to the electrode and demonstrated successful sensing of H2O2. Furthermore, to achieve detection of H2O2 in physiological conditions, CNPs were integrated with nanoporous gold (NPG) which exhibited anti-biofouling properties. The anti-biofouling property of NPG was investigated using electrochemical techniques and showed excellent signal retention in physiological concentration of albumin proteins. The novel study targets at developing robust enzyme free biosensor by integrating the detection ability of CNPs with the anti-biofouling activity of NPG based electrode.
Show less - Date Issued
- 2016
- Identifier
- CFE0006498, ucf:51404
- Format
- Document (PDF)
- PURL
- http://purl.flvc.org/ucf/fd/CFE0006498
- Title
- Liquid Crystal-Based Biosensors for the Detection of Bile Acids.
- Creator
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He, Sihui, Wu, Shintson, Kuebler, Stephen, Kik, Pieter, Fang, Jiyu, University of Central Florida
- Abstract / Description
-
Bile acids are physiologically important metabolites, which are synthesized in liver as the end products of cholesterol metabolism and then secreted into intestine. They are amphiphilic molecules which play a critical role in the digestion and absorption of fats and fat-soluble vitamins through emulsification. The concentration of bile acids is an indicator for liver function. Individual suffering from liver diseases has a sharp increase in bile acid concentrations. Hence, the concentration...
Show moreBile acids are physiologically important metabolites, which are synthesized in liver as the end products of cholesterol metabolism and then secreted into intestine. They are amphiphilic molecules which play a critical role in the digestion and absorption of fats and fat-soluble vitamins through emulsification. The concentration of bile acids is an indicator for liver function. Individual suffering from liver diseases has a sharp increase in bile acid concentrations. Hence, the concentration level of bile acids has long been used as a biomarker for the early diagnosis of intestinal and liver diseases.Conventional methods of bile acid detection such as chromatography-mass spectrometry and enzymatic reactions are complex and expensive. It is highly desired to have a simple, fast, and low-cost detection of bile acids that is available for self-testing or point-of-care testing. To achieve this goal, we develop a liquid crystal-based biosensor for the detection of bile acids. The sensor platform is based on the anchoring transition of liquid crystals (LCs) at the sodium dodecyl sulfate (SDS)-laden LC/aqueous interface for the detection of bile acids in aqueous solution. The first part of this dissertation focuses on the detection mechanism of bile acids. Our studies show that the displacement of SDS from the LC/aqueous interface by the competitive adsorption of bile acids induces a homeotropic-to-planar anchoring transition of the LC at the interface, providing an optical signature for the simple and rapid detection of bile acids. The adsorption of bile acids on the interface was found to follow Langmuir-Freundlich isotherm. The adsorption kinetics of different bile acids is compared. We find that both the number and position of hydroxyl groups of bile acids affect their adsorption kinetics. The different optical patterns of LC films formed by the adsorption of bile acids are also discussed. The second part of this dissertation studies the effect of solution conditions, surfactants, and liquid crystals on the detection limit of the LC-based biosensor for bile acids. Low pH and high ionic strength in the aqueous solution can reduce the electrostatic interaction between SDS and bile acids, which leads to a decreased detection limit. Surfactants with smaller headgroup and lower packing density also help to reduce the detection limit. To further reduce the detection limit, we investigate the effect of LC structures and find that LCs with a shorter chain length give lower detection limits. Also, by substituting a phenyl ring with a cyclohexane ring, we find that the detection limit is further reduced due to the decrease of the interaction between the phenyl rings of LCs. By mixing different LCs together, the detection limit can be linearly tuned from 160 (&)#181;M to 1.5 (&)#181;M, which is comparable to the traditional methods. But the LC-based biosensors have much simpler design and manufacture process.The third part of this dissertation is to apply this LC-based biosensor to the detection of urinary bile acids. We test the influence of several potential interfering species such as urea, creatinine, uric acid and ascorbic acid by conducting experiments in synthetic urine. By adjusting the concentration of SDS, we are able to eliminate the impact of those interfering species, and demonstrate that the LC-based biosensors can selectively detect urinary bile acids in human urine, suggesting its potential for screening liver dysfunctions. The final part of this dissertation is to investigate the application of LC-based biosensors in detecting the lipolysis process by porcine pancreatic lipase (PPL). It has been a long-standing argument over the role of bile salts on the activity of PPL. Thus, we study the time course of the hydrolysis of phospholipid L-dipalmitoylphosphatidylcholine (L-DPPC) by PPL at LC/aqueous interface. The hydrolysis of L-DPPC leads to a homeotropic-to-tilted anchoring transition of the LC at the interface, which allows the hydrolysis process to be monitored by a polarizing optical microscope. The microscopy image analysis reveals a lag-burst kinetics where a lag phase is followed by a burst phase. The effect of bile acids on these two phases is studied. We find that the activity of PPL both in the presence and absence of colipase can be improved by increasing the concentration of bile acids. The improvement becomes more distinct in the presence of colipase.
Show less - Date Issued
- 2015
- Identifier
- CFE0005804, ucf:50028
- Format
- Document (PDF)
- PURL
- http://purl.flvc.org/ucf/fd/CFE0005804
- Title
- LITERATURE REVIEW ON THE USE OF NUCLEIC ACID-BASED LOGIC GATES FOR THE DETECTION OF HUMAN DISEASES.
- Creator
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Blanco Martinez, Enrique J, Kolpashchikov, Dmitry, University of Central Florida
- Abstract / Description
-
Conventional methods for diagnosis of human disease are, at times, limited in different regards including time requirement, either experimental or data processing, sensitivity, and selectivity. It is then that a Point of Care Criteria, which considers the true utility and usefulness of the device, is employed to propose new diagnostic devices capable of overcoming the aforementioned shortcomings of conventional tools. Nucleic acid, characterized for its predictable base-pairing nature, is...
Show moreConventional methods for diagnosis of human disease are, at times, limited in different regards including time requirement, either experimental or data processing, sensitivity, and selectivity. It is then that a Point of Care Criteria, which considers the true utility and usefulness of the device, is employed to propose new diagnostic devices capable of overcoming the aforementioned shortcomings of conventional tools. Nucleic acid, characterized for its predictable base-pairing nature, is considered to be a highly-selective, yet greatly modifiable device. Its behavior is then described through Boolean Logic, where "true" or "false" outputs are mathematically described as "1" and "0", respectively. This mathematical approach is then referred to as Logic Gates, where outputs can be predicted based on satisfied environmental conditions. The mechanisms, capable of exhibiting Logic Gate behavior, are described.
Show less - Date Issued
- 2017
- Identifier
- CFH2000256, ucf:46006
- Format
- Document (PDF)
- PURL
- http://purl.flvc.org/ucf/fd/CFH2000256
- Title
- INTEGRATED OPTICAL SPR (SURFACE PLASMON RESONANCE) SENSOR BASED ON OPTOELECTRONIC PLATFORM.
- Creator
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Bang, Hyungseok, LiKamWa, Patrick, University of Central Florida
- Abstract / Description
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Current major demands in SPR sensor development are system miniaturization and throughput improvement. Structuring an array of integrated optical SPR sensor heads on a semiconductor based optoelectronic platform could be a promising solution for those issues, since integrated optical waveguides have highly miniaturized dimension and the optoelectronic platform enables on-chip optical-to-electrical signal conversion. Utilizing a semiconductor based platform to achieve optoelectronic...
Show moreCurrent major demands in SPR sensor development are system miniaturization and throughput improvement. Structuring an array of integrated optical SPR sensor heads on a semiconductor based optoelectronic platform could be a promising solution for those issues, since integrated optical waveguides have highly miniaturized dimension and the optoelectronic platform enables on-chip optical-to-electrical signal conversion. Utilizing a semiconductor based platform to achieve optoelectronic functionality poses requirements to the senor head; the sensor head needs to have reasonably small size while it should have reasonable sensitivity and fabrication tolerance. This research proposes a novel type of SPR sensor head and demonstrates a fabricated device with an array of integrated optical SPR sensor heads endowed with optoelectronic functionality. The novel integrated optical SPR sensor head relies on mode conversion efficiency for its operational principle. The beauty of this type of sensor head is it can produce clear contrast in SPR spectrum with a highly miniaturized and simple structure, in contrast to several-millimeter-scale conventional absorption type or interferometer type sensor heads. The integrated optical SPR sensor with optoelectronic functionality has been realized by structuring a dielectric waveguide based SPR sensor head on a photodetector-integrated semiconductor substrate. A large number of unit sensors have been fabricated on a substrate with a batch fabrication process, which promises a high throughput SPR sensor system or low-priced disposable sensors.
Show less - Date Issued
- 2008
- Identifier
- CFE0002312, ucf:47841
- Format
- Document (PDF)
- PURL
- http://purl.flvc.org/ucf/fd/CFE0002312
- Title
- Fabrication and Investigation of an enzyme-free, Nanoparticle-based Biosensor for Hydrogen Peroxide determination.
- Creator
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Neal, Craig, Seal, Sudipta, Cho, Hyoung Jin, Florczyk, Stephen, University of Central Florida
- Abstract / Description
-
Electrochemical biosensors often employ enzymes as detection elements. These sensors are highly selective towards target analytes, however the scope of their application is limited by the poor stability of the enzyme. In this study, multi-valent inorganic cerium oxide nanoparticles were used as detection elements for the analysis of hydrogen peroxide. The electrochemical response of the cerium oxide towards hydrogen peroxide analyte is defined through cyclic voltammetry and chronoamperometry....
Show moreElectrochemical biosensors often employ enzymes as detection elements. These sensors are highly selective towards target analytes, however the scope of their application is limited by the poor stability of the enzyme. In this study, multi-valent inorganic cerium oxide nanoparticles were used as detection elements for the analysis of hydrogen peroxide. The electrochemical response of the cerium oxide towards hydrogen peroxide analyte is defined through cyclic voltammetry and chronoamperometry. This response was found to be dependent on nanoparticle Ce3+:Ce4+ redox state ratio and this property is exploited to fabricate a biosensor. As produced, the biosensor demonstrated sensitivity at picomolar analyte concentrations. Further, the sensitivity of the electrode is stable across a range of temperatures and pH's which inhibit the function of standard enzyme-based sensors. Additionally, the produced sensor retained function in sheep serum demonstrating the high selectivity and robustness of the sensor.
Show less - Date Issued
- 2016
- Identifier
- CFE0006362, ucf:51540
- Format
- Document (PDF)
- PURL
- http://purl.flvc.org/ucf/fd/CFE0006362
- Title
- The Study of Physiochemical Properties of Cerium Oxide Nanoparticles and its Application in Biosensors.
- Creator
-
Barkam, Swetha, Seal, Sudipta, Heinrich, Helge, Gaume, Romain, University of Central Florida
- Abstract / Description
-
Biosensors continue to get smaller and faster with the advancement in nanotechnology through the use of nanomaterials to achieve high sensitivity and selectivity. However, the continued reliance on biomolecules or enzymes in the biosensor assembly poses the problem of reproducibility, storage and complexity. This dissertation research address some of the challenges by investigating the physiochemical properties of nanoparticles to understand its interaction with biological systems and develop...
Show moreBiosensors continue to get smaller and faster with the advancement in nanotechnology through the use of nanomaterials to achieve high sensitivity and selectivity. However, the continued reliance on biomolecules or enzymes in the biosensor assembly poses the problem of reproducibility, storage and complexity. This dissertation research address some of the challenges by investigating the physiochemical properties of nanoparticles to understand its interaction with biological systems and develop enzyme free biosensors. In this study, we have demonstrated a novel strategy to integrate cerium oxide nanoparticles (CNPs) as an efficient transducer through rigorous screening for developing enzyme/label free biosensors for detecting analytes such as dopamine associated with neurodegenerative diseases and limonin for fruit quality management. CNPs have been proven to exhibit antioxidant properties attributed to its dynamic change in surface oxidation states (Ce4+ to Ce3+ and vice versa) mediated at the oxygen vacancies on the surface of the CNPs. It is also well-established that nanoparticles are resourceful novel materials with a plethora of applications in the field of nanomedicine.It is of significant importance to study the changes in physiochemical properties of different synthesized CNPs for effective use in biomedical applications. In one of the studies, the effects of different anions in the precursor of the cerium salts used for synthesizing CNPs using the same synthesis method, were extensively studied. It has been demonstrated that the physicochemical properties such as dispersion stability, hydrodynamic size, and the signature surface chemistry, antioxidant catalytic activity, oxidation potentials of different CNPs have been significantly altered with the change of anions in the precursor salts. . The increased antioxidant property of CNPs prepared using the precursor salts containing NO3(&)#175; and Cl(&)#175; ions have been extensively studied using in-situ UV-Visible spectroscopy which reveal that the change in oxidation potentials of CNPs with the change in concentration of anions. Thus, this work demonstrated that the physicochemical and antioxidant properties of CNPs can be tuned by anions of the precursor during the synthesis process.After standardizing the synthesis process, CNPs have been immobilized on highly ordered polymer nanopillars to develop an optical sensor for dopamine detection. Dopamine, is one of the main neurotransmitters which plays a significant role in central nervous system and its deficiency leads to neurological disorders such as Parkinson's disease, schizophrenia etc. Current biosensors in the literature use invasive detection techniques and lacks sensitivity to detect physiological clinically relevant concentrations of dopamine. The interaction between CNPs and dopamine have been extensively studied using UV-visible spectro-electrochemical studies to achieve the right surface chemistry (35-70% Ce4+). The sensor exhibits high sensitivity (1fM detection in simulated body fluid), high selectivity (in acetic acid, sheep plasma) and increased robustness with several cycles of usage.Furthermore, we have developed a CNPs based biosensor by integrating it on a transistor platform for improved sensitivity and better adhesion by immobilizing in silk fibroin matrix. In the final study, CNPs integrated in silk fibroin (SF) polymer electrospun nanofibers incorporated on an organic electrochemical transistor platform, is used to develop a limonin sensor. It has been established that the concentration of limonin in citric fruit predicts the quality in terms of bitter taste from the HLB bacteria infected fruits. A unique in-house electrospinning set-up using drum as collector was used to develop SF (extracted from cocoon) nanofibers used as CNP (synthesized in-situ in fibers) transducer carrier, both of which have a specific interaction with limonin. This novel biosensor has exhibited high sensitivity (100nM in PBS) and selectivity (citric acid, sugar etc.) with improved robustness in terms of reuse. The broader impact of the study is to develop holistic diagnostic non-invasive biosensors that can directly be used to detect the analytes using samples from humans and/or on field for fruit quality determination, which is a huge stepping stone in the advancement of nanotechnology based biosensors. This will fuel future generation of enzyme free biosensors which can utilize similar concepts for the detection of other analytes. The biosensor could be printed on a flexible substrate to advance wearable smart biosensor and could eventually enable users to wirelessly monitor the analyte concentrations using smartphones.
Show less - Date Issued
- 2017
- Identifier
- CFE0006931, ucf:51662
- Format
- Document (PDF)
- PURL
- http://purl.flvc.org/ucf/fd/CFE0006931
- Title
- Self-Assembled Two-Component Organic Tubes: Structures and Applications.
- Creator
-
Liang, Wenlang, Fang, Jiyu, Huo, Qun, Deng, Weiwei, University of Central Florida
- Abstract / Description
-
Bile acids are physiologically important metabolites, which are synthesized in liver as the end products of cholesterol metabolism and then secreted into the intestines. They play a critical role in the digestion and absorption of fats and fat-soluble vitamins through emulsifications. The amphipathic and chiral nature of bile acids makes their unique building blocks for assembling supramolecular structures including vesicles, fibers, ribbons and hollow tubes. Lithocholic acid (LCA) is a...
Show moreBile acids are physiologically important metabolites, which are synthesized in liver as the end products of cholesterol metabolism and then secreted into the intestines. They play a critical role in the digestion and absorption of fats and fat-soluble vitamins through emulsifications. The amphipathic and chiral nature of bile acids makes their unique building blocks for assembling supramolecular structures including vesicles, fibers, ribbons and hollow tubes. Lithocholic acid (LCA) is a secondary bile acid. Our studies show LCA can self-assemble into helical tubes in aqueous solution by the linear aggregation and fusion of vesicles. The objective of this dissertation is to tune the structure of helical tubes and functionalize them by the co-assembly of ionic LCA and cationic cetyltrimethylammonium bromide (CTAB) and ionic LCA and cationic cyanine dye (CD), respectively. The first part of this dissertation focuses on the ionic-assembly of LCA and CTAB to synthesize the helical tubes with varied diameters and pitches. Our studies show that LCA and CTAB can self-assemble into helical tubes in NH4OH aqueous solution. The diameter of the helical tubes can be changed by adjusting the molar ratio of LCA and CTAB. The pitch of the helical tubes can be tuned by varying NH4OH concentrations. Differential scanning calorimetry studies indicate that there is a homogeneous composition distribution in the LCA/CTAB helical tubes. X-ray diffraction analysis studies show that the helical tubes have multibilayer walls with an average d-spacing of 4.11nm. We demonstrate that the helical tubes with varied diameters and pitches can be transformed into helical silica through the sol-gel transcription of tetraethoxysilane (TEOS). The second part of this dissertation is to use the ionic self-assembly of LCA and CD to design light-harvesting tubes by mimicking green sulfur bacteria that are known to be a highly efficient photosynthesizer. X-ray diffraction and optical spectra show that LCA and CD can co-assemble into J- or H-aggregate tubes, depending the condition under which the self-assembly occurs. We demonstrate the feasibility of using the J-aggregate nanotubes in the sensitive and selective detection of mercury (II) ions by the photoinduced electron transfer under sunlight. The presence of mercury (II) ions in aqueous solution could be detected for concentrations as low as 10 pM.
Show less - Date Issued
- 2013
- Identifier
- CFE0005201, ucf:50635
- Format
- Document (PDF)
- PURL
- http://purl.flvc.org/ucf/fd/CFE0005201
- Title
- FUNDAMENTAL ASPECTS OF REGENERATIVE CERIUM OXIDE NANOPARTICLES AND THEIR APPLICATIONS IN NANOBIOTECHNOLOGY.
- Creator
-
Patil, Swanand, Seal, Sudipta, University of Central Florida
- Abstract / Description
-
Cerium oxide has been used extensively for various applications over the past two decades. The use of cerium oxide nanoparticles is beneficial in present applications and can open avenues for future applications. The present study utilizes the microemulsion technique to synthesize uniformly distributed cerium oxide nanoparticles. The same technique was also used to synthesize cerium oxide nanoparticles doped with trivalent elements (La and Nd). The fundamental study of cerium oxide...
Show moreCerium oxide has been used extensively for various applications over the past two decades. The use of cerium oxide nanoparticles is beneficial in present applications and can open avenues for future applications. The present study utilizes the microemulsion technique to synthesize uniformly distributed cerium oxide nanoparticles. The same technique was also used to synthesize cerium oxide nanoparticles doped with trivalent elements (La and Nd). The fundamental study of cerium oxide nanoparticles identified variations in properties as a function of particle size and also due to doping with trivalent elements (La and Nd). It was found that the lattice parameter of cerium oxide nanoparticles increases with decrease in particle size. Also Raman allowed mode shift to lower energies and the peak at 464 cm-1 becomes broader and asymmetric. The size dependent changes in cerium oxide were correlated to increase in oxygen vacancy concentration in the cerium oxide lattice. The doping of cerium oxide nanoparticles with trivalent elements introduces more oxygen vacancies and expands the cerium oxide lattice further (in addition to the lattice expansion due to the size effect). The lattice expansion is greater for La-doped cerium oxide nanoparticles compared to Nd-doping due to the larger ionic radius of La compared to Nd, the lattice expansion is directly proportional to the dopant concentration. The synthesized cerium oxide nanoparticles were used to develop an electrochemical biosensor of hydrogen peroxide (H2O2). The sensor was useful to detect H2O2 concentrations as low as 1µM in water. Also the preliminary testing of the sensor on tomato stem and leaf extracts indicated that the sensor can be used in practical applications such as plant physiological studies etc. The nanomolar concentrations of cerium oxide nanoparticles were also found to be useful in decreasing ROS (reactive oxygen species) mediated cellular damages in various in vitro cell cultures. Cerium oxide nanoparticles reduced the cellular damages to the normal breast epithelial cell line (CRL 8798) induced by X-rays and to the Keratinocyte cell line induced by UV irradiation. Cerium oxide nanoparticles were also found to be neuroprotective to adult rat spinal cord and retinal neurons. We propose that cerium oxide nanoparticles act as free radical scavenger (via redox reactions on its surface) to decrease the ROS induced cellular damages. Additionally, UV-visible spectroscopic studies indicated that cerium oxide nanoparticles possess auto-regenerative property by switching its oxidation state between Ce3+ and Ce4+. The auto-regenerative antioxidant property of these nanoparticles appears to be a key component in all the biological applications discussed in the present study.
Show less - Date Issued
- 2006
- Identifier
- CFE0001271, ucf:46932
- Format
- Document (PDF)
- PURL
- http://purl.flvc.org/ucf/fd/CFE0001271
- Title
- USING ANTENNA TILE-ASSISTED SUBSTRATE DELIVERY TO IMPROVE THE DETECTION LIMITS OF DEOXYRIBOZYME BIOSENSORS.
- Creator
-
Cox, Amanda, Kolpashchikov, Dmitry, University of Central Florida
- Abstract / Description
-
One common limitation of enzymatic reactions is the diffusion of a substrate to the enzyme active site and/or the release of the reaction products. These reactions are known as diffusion-controlled. Overcoming this limitation may enable faster catalytic rates, which in the case of catalytic biosensors can potentially lower limits of detection of specific analyte. Here we created an artificial system to enable deoxyribozyme (Dz) 10-23 based biosensor to overcome its diffusion limit. The sensor...
Show moreOne common limitation of enzymatic reactions is the diffusion of a substrate to the enzyme active site and/or the release of the reaction products. These reactions are known as diffusion-controlled. Overcoming this limitation may enable faster catalytic rates, which in the case of catalytic biosensors can potentially lower limits of detection of specific analyte. Here we created an artificial system to enable deoxyribozyme (Dz) 10-23 based biosensor to overcome its diffusion limit. The sensor consists of the two probe strands, which bind to the analyzed nucleic acid by Watson-Crick base pairs and, upon binding re-form the catalytic core of Dz 10-23. The activated Dz 10-23 cleaves the fluorophore and quencher-labeled DNA-RNA substrate which separates the fluorophore from the quencher thus producing high fluorescent signal. This system uses a Dz 10-23 biosensor strand associated to a DNA antenna tile, which captures the fluorogenic substrate and channels it to the reaction center where the Dz 10-23 cleaves the substrate. DNA antenna tile captures fluorogenic substrate and delivers it to the activated Dz 10-23 core. This allows for lower levels of analyte to be detected without compromising the specificity of the biosensor. The results of this experiment demonstrated that using DNA antenna, we can create a synthetic environment around the Dz 10-23 biosensor to increase its efficiency and allow for lower levels of analyte to be detected without using amplification techniques like PCR.
Show less - Date Issued
- 2015
- Identifier
- CFH0004887, ucf:45432
- Format
- Document (PDF)
- PURL
- http://purl.flvc.org/ucf/fd/CFH0004887
- Title
- A Universal Electrochemical Biosensor for the Detection of Nucleic Acids based on a Four-Way Junction Structure.
- Creator
-
Mills, Dawn, Chumbimuni Torres, Karin, Kolpashchikov, Dmitry, Campiglia, Andres, Dupras, Tosha, Tetard, Laurene, University of Central Florida
- Abstract / Description
-
Electrochemical hybridization sensors have been explored extensively for analysis of specific nucleic acids. However, commercialization of the platform is hindered by the need for attachment of separate oligonucleotide probes complementary to a RNA or DNA target to an electrode's surface. This dissertation demonstrates that a single probe can be used to analyze several nucleic acid targets of different lengths with high selectivity, low cost and can be regenerated in 30 seconds by a simple...
Show moreElectrochemical hybridization sensors have been explored extensively for analysis of specific nucleic acids. However, commercialization of the platform is hindered by the need for attachment of separate oligonucleotide probes complementary to a RNA or DNA target to an electrode's surface. This dissertation demonstrates that a single probe can be used to analyze several nucleic acid targets of different lengths with high selectivity, low cost and can be regenerated in 30 seconds by a simple water rinse. The universal electrochemical four-way junction (4J)-forming (UE4J) sensor consists of a universal DNA stem-loop (USL) probe attached to the electrode's surface and two adaptor strands (m and f) which hybridize to the USL probe and the analyte to form a 4J structure. The UE4J sensor enables a high selectivity by recognition of a single base substitution, even at room temperature. The sensor was monitored with voltammetry and electrochemical impedance spectroscopy using different redox labeling strategies and optimized using synthetic nucleic acid sequences. After the sensor was optimized and fully characterized, it was modified for the detection of the Zika virus. The UE4J sensor presented here opens a venue for a re-useable universal platform that can be adopted at low cost for the analysis of potentially any DNA or RNA targets.
Show less - Date Issued
- 2017
- Identifier
- CFE0007290, ucf:52146
- Format
- Document (PDF)
- PURL
- http://purl.flvc.org/ucf/fd/CFE0007290
- Title
- THEORETICAL TAILORING OF PERFORATED THIN SILVER FILMS FOR AFFINITY SURFACE PLASMON RESONANCE BIOSENSOR APPLICATIONS.
- Creator
-
Gongora Jr., Renan, Zou, Shengli, University of Central Florida
- Abstract / Description
-
Metallic films, in conjunction with biochemical-targeted probes, are expected to provide early diagnosis, targeted therapy and non-invasive monitoring for epidemiology applications. The resonance wavelength peaks, both plasmonic and Wood-Rayleigh Anomalies (WRAs), in the scattering spectra are affected by the metallic architecture. As of today, much research has been devoted to extinction efficiency in the plasmonic region. However, Wood Rayleigh Anomalies (WRAs) typically occur at...
Show moreMetallic films, in conjunction with biochemical-targeted probes, are expected to provide early diagnosis, targeted therapy and non-invasive monitoring for epidemiology applications. The resonance wavelength peaks, both plasmonic and Wood-Rayleigh Anomalies (WRAs), in the scattering spectra are affected by the metallic architecture. As of today, much research has been devoted to extinction efficiency in the plasmonic region. However, Wood Rayleigh Anomalies (WRAs) typically occur at wavelengths associated with the periodic distance of the structures. A significant number of papers have already focused on the plasmonic region of the visible spectrum, but a less explored area of research was presented here; the desired resonance wavelength region was 400-500nm, corresponding to the WRA for the silver film with perforated hole with a periodic distance of 400nm. Simulations obtained from the discrete dipole approximation (DDA) method, show sharp spectral bands (either high or low scattering efficiencies) in both wavelength regions of the visible spectrum simulated from Ag film with cylindrical hole arrays In addition, surprising results were obtained in the parallel scattering spectra,where the electric field is contained in the XY plane, when the angle between the metallic surface and the incident light was adjusted to 14 degrees; a bathochromic shift was observed for the WRA peak suggesting a hybrid resonance mode. Metallic films have the potential to be used in instrumental techniques for use as sensors, i.e. surface plasmon resonance affinity biosensors, but are not limited to such instrumental techniques. Although the research here was aimed towards affinity biosensors, other sensory designs can benefit from the optimized Ag film motifs. The intent of the study was to elucidate metal film motifs, when incorporated into instrumental analysis, allowing the quantification of genetic material in the visible region. Any research group that routinely benefits from quantification of various analytes in solution matrices will also benefit from this study, as there are a bewildering number of instrumental sensory methods and setups available.
Show less - Date Issued
- 2014
- Identifier
- CFH0004538, ucf:45155
- Format
- Document (PDF)
- PURL
- http://purl.flvc.org/ucf/fd/CFH0004538
- Title
- Photoactivatable Organic and Inorganic Nanoparticles in Cancer Therapeutics and Biosensing.
- Creator
-
Mathew, Mona, Gesquiere, Andre, Hickman, James, Ye, Jingdong, Campiglia, Andres, Schoenfeld, Winston, University of Central Florida
- Abstract / Description
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In photodynamic therapy a photosensitizer drug is administered and is irradiated with light. Upon absorption of light the photosensitizer goes into its triplet state and transfers energy or an electron to oxygen to form reactive oxygen species (ROS). These ROS react with biomolecules in cells leading to cell damage and cell death. PDT has interested many researchers because of its non-invasiveness as compared to surgery, it leaves little to no scars, it is time and cost effective, it has...
Show moreIn photodynamic therapy a photosensitizer drug is administered and is irradiated with light. Upon absorption of light the photosensitizer goes into its triplet state and transfers energy or an electron to oxygen to form reactive oxygen species (ROS). These ROS react with biomolecules in cells leading to cell damage and cell death. PDT has interested many researchers because of its non-invasiveness as compared to surgery, it leaves little to no scars, it is time and cost effective, it has potential for targeted treatment, and can be repeated as needed. Different photosensitizers such as porphyrines, chlorophylls, and dyes have been used in PDT to treat various cancers, skin diseases, aging and sun-damaged skin. These second generation sensitizers have yielded reduced skin sensitivity and improved extinction coefficients (up to ~ 105 L mol-1 cm-1). While PDT based on small molecule photosensitizers has shown great promise, several problems remain unsolved. The main issues with current sensitizers are (i) hydrophobicity leading to aggregation in aqueous media resulting in reduced efficacy and potential toxicity, (ii) dark toxicity of photosensitizers, (iii) non-selectivity towards malignant tissue resulting in prolonged cutaneous photosensitivity and damage to healthy tissue, (iv) limited light absorption efficiency, and (v) a lack of understanding of where the photosensitizer ends up in the tissue. In this dissertation research program, these issues were addressed by the development of conducting polymer nanoparticles as a next generation of photosensitizers. This choice was motivated by the fact that conducting polymers have large extinction coefficients ((>) 107 L mol-1 cm-1), are able to undergo intersystem crossing to the triplet state, and have triplet energies that are close to that of oxygen. It was therefore hypothesized that such polymers could be effective at generating ROS due to the large excitation rate that can be generated. Conducting polymer nanoparticles (CPNPs) composed of the conducting polymer poly[2-methoxy-5-(2-ethylhexyl-oxy)-p-phenylenevinylene] (MEH-PPV) were fabricated and studied in-vitro for their potential in PDT application. Although not fully selective, the nanoparticles exhibited a strong bias to the cancer cells. The formation of ROS was proven in-vitro by staining of the cells with CellROX Green Reagent, after which PDT results were quantified by MTT assays. Cell mortality was observed to scale with nanoparticle dosage and light dosage. Based on these promising results the MEH-PPV nanoparticles were developed further to allow for surface functionalization, with the aim of targeting these NPs to cancer cell lines. For this work targeting of cancers that overexpress folate receptors (FR) were considered. The functionalized nanoparticles (FNPs) were studied in OVCAR3 (ovarian cancer cell line) as FR+, MIA PaCa2 (pancreatic cell line) as FR-, and A549 (lung cancer cell line) having marginal FR expression. Complete selectivity of the FNPs towards the FR+ cell line was found. Quantification of PDT results by MTS assays and flow cytometry show that PDT treatment was fully selective to the FR+ cell line (OVCAR3). No cell mortality was observed for the other cell lines studied here within experimental error. Finally, the issue of confirming and quantifying small molecule drug delivery to diseased tissue was tackled by developing quantum dot (Qdot) biosensors with the aim of achieving fluorescence reporting of intracellular small molecule/drug delivery. For fluorescence reporting prior expertise in control of the fluorescence state of Qdots was employed, where redox active ligands can place the Qdot in a quenched OFF state. Ligand attachment was accomplished by disulfide linker chemistry. This chemistry is reversible in the presence of sulfur reducing biomolecules, resulting in Qdots in a brightly fluorescent ON state. Glutathione (GSH) is such a biomolecule that is present in the intracellular environment. Experimental in-vitro data shows that this design was successfully implemented.
Show less - Date Issued
- 2014
- Identifier
- CFE0005839, ucf:50923
- Format
- Document (PDF)
- PURL
- http://purl.flvc.org/ucf/fd/CFE0005839
- Title
- Nonlinear dynamic modeling, simulation and characterization of the mesoscale neuron-electrode interface.
- Creator
-
Thakore, Vaibhav, Hickman, James, Mucciolo, Eduardo, Rahman, Talat, Johnson, Michael, Behal, Aman, Molnar, Peter, University of Central Florida
- Abstract / Description
-
Extracellular neuroelectronic interfacing has important applications in the fields of neural prosthetics, biological computation and whole-cell biosensing for drug screening and toxin detection. While the field of neuroelectronic interfacing holds great promise, the recording of high-fidelity signals from extracellular devices has long suffered from the problem of low signal-to-noise ratios and changes in signal shapes due to the presence of highly dispersive dielectric medium in the neuron...
Show moreExtracellular neuroelectronic interfacing has important applications in the fields of neural prosthetics, biological computation and whole-cell biosensing for drug screening and toxin detection. While the field of neuroelectronic interfacing holds great promise, the recording of high-fidelity signals from extracellular devices has long suffered from the problem of low signal-to-noise ratios and changes in signal shapes due to the presence of highly dispersive dielectric medium in the neuron-microelectrode cleft. This has made it difficult to correlate the extracellularly recorded signals with the intracellular signals recorded using conventional patch-clamp electrophysiology. For bringing about an improvement in the signal-to-noise ratio of the signals recorded on the extracellular microelectrodes and to explore strategies for engineering the neuron-electrode interface there exists a need to model, simulate and characterize the cell-sensor interface to better understand the mechanism of signal transduction across the interface. Efforts to date for modeling the neuron-electrode interface have primarily focused on the use of point or area contact linear equivalent circuit models for a description of the interface with an assumption of passive linearity for the dynamics of the interfacial medium in the cell-electrode cleft. In this dissertation, results are presented from a nonlinear dynamic characterization of the neuroelectronic junction based on Volterra-Wiener modeling which showed that the process of signal transduction at the interface may have nonlinear contributions from the interfacial medium. An optimization based study of linear equivalent circuit models for representing signals recorded at the neuron-electrode interface subsequently proved conclusively that the process of signal transduction across the interface is indeed nonlinear. Following this a theoretical framework for the extraction of the complex nonlinear material parameters of the interfacial medium like the dielectric permittivity, conductivity and diffusivity tensors based on dynamic nonlinear Volterra-Wiener modeling was developed. Within this framework, the use of Gaussian bandlimited white noise for nonlinear impedance spectroscopy was shown to offer considerable advantages over the use of sinusoidal inputs for nonlinear harmonic analysis currently employed in impedance characterization of nonlinear electrochemical systems. Signal transduction at the neuron-microelectrode interface is mediated by the interfacial medium confined to a thin cleft with thickness on the scale of 20-110 nm giving rise to Knudsen numbers (ratio of mean free path to characteristic system length) in the range of 0.015 and 0.003 for ionic electrodiffusion. At these Knudsen numbers, the continuum assumptions made in the use of Poisson-Nernst-Planck system of equations for modeling ionic electrodiffusion are not valid. Therefore, a lattice Boltzmann method (LBM) based multiphysics solver suitable for modeling ionic electrodiffusion at the mesoscale neuron-microelectrode interface was developed. Additionally, a molecular speed dependent relaxation time was proposed for use in the lattice Boltzmann equation. Such a relaxation time holds promise for enhancing the numerical stability of lattice Boltzmann algorithms as it helped recover a physically correct description of microscopic phenomena related to particle collisions governed by their local density on the lattice. Next, using this multiphysics solver simulations were carried out for the charge relaxation dynamics of an electrolytic nanocapacitor with the intention of ultimately employing it for a simulation of the capacitive coupling between the neuron and the planar microelectrode on a microelectrode array (MEA). Simulations of the charge relaxation dynamics for a step potential applied at t = 0 to the capacitor electrodes were carried out for varying conditions of electric double layer (EDL) overlap, solvent viscosity, electrode spacing and ratio of cation to anion diffusivity. For a large EDL overlap, an anomalous plasma-like collective behavior of oscillating ions at a frequency much lower than the plasma frequency of the electrolyte was observed and as such it appears to be purely an effect of nanoscale confinement. Results from these simulations are then discussed in the context of the dynamics of the interfacial medium in the neuron-microelectrode cleft. In conclusion, a synergistic approach to engineering the neuron-microelectrode interface is outlined through a use of the nonlinear dynamic modeling, simulation and characterization tools developed as part of this dissertation research.
Show less - Date Issued
- 2012
- Identifier
- CFE0004797, ucf:49718
- Format
- Document (PDF)
- PURL
- http://purl.flvc.org/ucf/fd/CFE0004797
