Matching Items (22)

PEGylation of DNA Nanostructures Using Uncatalyzed Click Chemistry

Description

Using DNA nanotechnology a library of structures of various geometries have been built; these structures are modified chemically and/or enzymatically at nanometer precisions. With DNA being chemically very stable, these

Using DNA nanotechnology a library of structures of various geometries have been built; these structures are modified chemically and/or enzymatically at nanometer precisions. With DNA being chemically very stable, these structures can be functionalized through an abundance of well-established protocols. Additionally, they can be used for various biological and medicinal purposes, such as drug delivery. For in vivo applications, the DNA nanostructures must have a long circulation life in the bloodstream; otherwise, they could be easily excreted shortly after entry. One way of making these nanostructures long lasting in the blood is to cover them with the biocompatible polymer, polyethylene glycol (PEG). Adding DNA to PEG before forming structures has been found to interfere in the hybridization of the DNA in the structure, resulting in formation of deformed structures. In this study we have developed a new methodology based on "click chemistry" (CC) to modify the surface of DNA nanostructures with PEG after they are formed. These structures can then be used for in vivo studies and potential applications in the future.

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Created

Date Created
  • 2015-05

Development and Design of DNA Origami Nanostructures for Single Cell Analysis of Paired γδ TCR mRNA

Description

Efforts to quantify the diversity of the T cell repertoire have generally been unsuccessful because not all factors accounting for diversity have been considered. In order to get an accurate

Efforts to quantify the diversity of the T cell repertoire have generally been unsuccessful because not all factors accounting for diversity have been considered. In order to get an accurate representation of the T cell repertoire, one must incorporate analysis of germline gene diversity, diversity from somatic recombination, joining diversity from N- and P- nucleotides, and TCR chain pairing diversity. Because of advances in high-throughput sequencing techniques, estimates have been able to account for diversity from TCR genes. However the ability to account for chain pairing diversity has been more difficult. In order to do so, single cell sorting techniques must be employed. These techniques, though effective, are time consuming and expensive. For this reason, no large-scale analyses have been done on the immune repertoires using these techniques. In this study, we propose a novel method for linking the two TCR chain sequences from an individual cell. DNA origami nanostructure technology is employed to capture and bind the TCRγ and TCRδ chain mRNA inside individual cells using probe strands complementary to the C-region of those sequences. We then use a dual-primer RT and ligation molecular strategy to link the two sequences together. The result is a single amplicon containing the CDR3 region of the TCRγ and TCRδ. This amplicon can then be easily PCR amplified using sequence specific primers, and sequenced. DNA origami nanostructures offer a rapid, cost-effective method alternative to conventional single cell sorting techniques, as both TCR mRNA can be captured on one origami molecule inside a single cell. At present, this study outlines a proof-of-principle analysis of the method to determine its functionality. Using known TCRγ and TCRδ sequences, the DNA origami and RT/PCR method was tested and resulting sequence data proved the effectiveness of the method. The original TCRγ and TCRδ sequences were linked together as a single amplicon containing both CDR3 regions of the genes. Thus, this method can be employed in further research to elucidate the γδ T cell repertoire. This technology is also easily adapted to any gene target or cell type and therefore presents a large opportunity to be used in other immune repertoire analysis and other immunological studies (such as the rapid identification and subsequent production of antibodies).

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Date Created
  • 2015-05

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ZnTe nanostructural synthesis for electronic and optoelectronic devices

Description

Zinc telluride (ZnTe) is an attractive II-VI compound semiconductor with a direct

bandgap of 2.26 eV that is used in many applications in optoelectronic devices. Compared

to the two dimensional (2D) thin-film

Zinc telluride (ZnTe) is an attractive II-VI compound semiconductor with a direct

bandgap of 2.26 eV that is used in many applications in optoelectronic devices. Compared

to the two dimensional (2D) thin-film semiconductors, one-dimensional (1D)

nanowires can have different electronic properties for potential novel applications.

In this work, we present the study of ZnTe nanowires (NWs) that are synthesized

through a simple vapor-liquid-solid (VLS) method. By controlling the presence or

the absence of Au catalysts and controlling the growth parameters such as growth

temperature, various growth morphologies of ZnTe, such as thin films and nanowires

can be obtained. The characterization of the ZnTe nanostructures and films was

performed using scanning electron microscope (SEM), energy-dispersive X-ray spectroscopy

(EDX), high- resolution transmission electron microscope (HRTEM), X-ray

diffraction (XRD), photoluminescence (PL), Raman spectroscopy and light scattering

measurement. After confirming the crystal purity of ZnTe, two-terminal diodes and

three-terminal transistors were fabricated with both nanowire and planar nano-sheet

configurations, in order to correlate the nanostructure geometry to device performance

including field effect mobility, Schottky barrier characteristics, and turn-on

characteristics. Additionally, optoelectronic properties such as photoconductive gain

and responsivity were compared against morphology. Finally, ZnTe was explored in

conjunction with ZnO in order to form type-II band alignment in a core-shell nanostructure.

Various characterization techniques including scanning electron microscopy,

energy-dispersive X-ray spectroscopy , x-ray diffraction, Raman spectroscopy, UV-vis

reflectance spectra and photoluminescence were used to investigate the modification

of ZnO/ZnTe core/shell structure properties. In PL spectra, the eliminated PL intensity

of ZnO wires is primarily attributed to the efficient charge transfer process

occurring between ZnO and ZnTe, due to the band alignment in the core/shell structure. Moreover, the result of UV-vis reflectance spectra corresponds to the band

gap energy of ZnO and ZnTe, respectively, which confirm that the sample consists of

ZnO/ZnTe core/shell structure of good quality.

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Created

Date Created
  • 2017

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Heterojunction and nanostructured photovoltaic device: theory and experiment

Description

A primary motivation of research in photovoltaic technology is to obtain higher efficiency photovoltaic devices at reduced cost of production so that solar electricity can be cost competitive. The majority

A primary motivation of research in photovoltaic technology is to obtain higher efficiency photovoltaic devices at reduced cost of production so that solar electricity can be cost competitive. The majority of photovoltaic technologies are based on p-n junction, with efficiency potential being much lower than the thermodynamic limits of individual technologies and thereby providing substantial scope for further improvements in efficiency. The thesis explores photovoltaic devices using new physical processes that rely on thin layers and are capable of attaining the thermodynamic limit of photovoltaic technology. Silicon heterostructure is one of the candidate technologies in which thin films induce a minority carrier collecting junction in silicon and the devices can achieve efficiency close to the thermodynamic limits of silicon technology. The thesis proposes and experimentally establishes a new theory explaining the operation of silicon heterostructure solar cells. The theory will assist in identifying the optimum properties of thin film materials for silicon heterostructure and help in design and characterization of the devices, along with aiding in developing new devices based on this technology. The efficiency potential of silicon heterostructure is constrained by the thermodynamic limit (31%) of single junction solar cell and is considerably lower than the limit of photovoltaic conversion (~ 80 %). A further improvement in photovoltaic conversion efficiency is possible by implementing a multiple quasi-fermi level system (MQFL). A MQFL allows the absorption of sub band gap photons with current being extracted at a higher band-gap, thereby allowing to overcome the efficiency limit of single junction devices. A MQFL can be realized either by thin epitaxial layers of alternating higher and lower band gap material with nearly lattice matched (quantum well) or highly lattice mismatched (quantum dot) structure. The thesis identifies the material combination for quantum well structure and calculates the absorption coefficient of a MQFl based on quantum well. GaAsSb (barrier)/InAs(dot) was identified as a candidate material for MQFL using quantum dot. The thesis explains the growth mechanism of GaAsSb and the optimization of GaAsSb and GaAs heterointerface.

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Created

Date Created
  • 2011

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Growth of InGaN nanorings via metal organic chemical vapor deposition

Description

III-Nitride nanostructures have been an active area of research recently due to their ability to tune their optoelectronic properties. Thus far work has been done on InGaN quantum dots, nanowires,

III-Nitride nanostructures have been an active area of research recently due to their ability to tune their optoelectronic properties. Thus far work has been done on InGaN quantum dots, nanowires, nanopillars, amongst other structures, but this research reports the creation of a new type of InGaN nanostructure, nanorings. Hexagonal InGaN nanorings were formed using Metal Organic Chemical Vapor Deposition through droplet epitaxy. The nanorings were thoroughly analyzed using x-ray diffraction, photoluminescence, electron microscopy, electron diffraction, and atomic force microscopy. Nanorings with high indium incorporation were achieved with indium content up to 50% that was then controlled using the growth time, temperature, In/Ga ratio and III/N ratio. The analysis showed that the nanoring shape is able to incorporate more indium than other nanostructures, due to the relaxing mechanism involved in the formation of the nanoring. The ideal conditions were determined to be growth of 30 second droplets with a growth time of 1 minute 30 seconds at 770 C to achieve the most well developed rings with the highest indium concentration.

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Date Created
  • 2012

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DNA tetrahedra as structural frameworks for catalytic centers

Description

The need for a renewable and sustainable light-driven energy source is the motivation for this work, which utilizes a challenging, yet practical and attainable bio-inspired approach to develop an artificial

The need for a renewable and sustainable light-driven energy source is the motivation for this work, which utilizes a challenging, yet practical and attainable bio-inspired approach to develop an artificial oxygen evolving complex, which builds upon the principles of the natural water splitting mechanism in oxygenic photosynthesis. In this work, a stable framework consisting of a three-dimensional DNA tetrahedron has been used for the design of a bio-mimic of the Oxygen-Evolving Complex (OEC) found in natural Photosystem II (PSII). PSII is a large protein complex that evolves all the oxygen in the atmosphere, but it cannot be used directly in artificial systems, as the light reactions lead to damage of one of Photosystem II's core proteins, D1, which has to be replaced every half hour in the presence of sunlight. The final goal of the project aims to build the catalytic center of the OEC, including the Mn4CaCl metal cluster and its protein environment in the stable DNA framework of a tetrahedron, which can subsequently be connected to a photo-stable artificial reaction center that performs light-induced charge separation. Regions of the peptide sequences containing Mn4CaCl ligation sites are implemented in the design of the aOEC (artificial oxygen-evolving complex) and are attached to sites within the tetrahedron to facilitate assembly. Crystals of the tetrahedron have been obtained, and X-ray crystallography has been used for characterization. As a proof of concept, metal-binding peptides have been coupled to the DNA tetrahedron which allowed metal-containing porphyrins, specifically Fe(III) meso-Tetra(4-sulfonatophenyl) porphyrin chloride, to be encapsulated inside the DNA-tetrahedron. The porphyrins were successfully assembled inside the tetrahedron through coordination of two terminal histidines from the orthogonally oriented peptides covalently attached to the DNA. The assembly has been characterized using Electron Paramagnetic Resonance (EPR), optical spectroscopy, Dynamic Light Scattering (DLS), and x-ray crystallography. The results reveal that the spin state of the metal, iron (III), switches during assembly from the high-spin state to low-spin state.

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Date Created
  • 2012

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Replication of DNA tetrahedron and higher-order self-assembly of DNA origami

Description

Deoxyribonucleic acid (DNA) has been treated as excellent building material for nanoscale construction because of its unique structural features. Its ability to self-assemble into predictable and addressable nanostructures distinguishes it

Deoxyribonucleic acid (DNA) has been treated as excellent building material for nanoscale construction because of its unique structural features. Its ability to self-assemble into predictable and addressable nanostructures distinguishes it from other materials. A large variety of DNA nanostructures have been constructed, providing scaffolds with nanometer precision to organize functional molecules. This dissertation focuses on developing biologically replicating DNA nanostructures to explore their biocompatibility for potential functions in cells, as well as studying the molecular behaviors of DNA origami tiles in higher-order self-assembly for constructing DNA nanostructures with large size and complexity. Presented here are a series of studies towards this goal. First, a single-stranded DNA tetrahedron was constructed and replicated in vivo with high efficiency and fidelity. This study indicated the compatibility between DNA nanostructures and biological systems, and suggested a feasible low-coast method to scale up the preparation of synthetic DNA. Next, the higher-order self-assembly of DNA origami tiles was systematically studied. It was demonstrated that the dimensional aspect ratio of origami tiles as well as the intertile connection design were essential in determining the assembled superstructures. Finally, the effects of DNA hairpin loops on the conformations of origami tiles as well as the higher-order assembled structures were demonstrated. The results would benefit the design and construction of large complex nanostructures.

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Date Created
  • 2012

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Growth and characterization of multisegment chalcogenide alloy nanostructures for photonic applications in a wide spectral range

Description

In this dissertation, I described my research on the growth and characterization of various nanostructures, such as nanowires, nanobelts and nanosheets, of different semiconductors in a Chemical Vapor Deposition (CVD)

In this dissertation, I described my research on the growth and characterization of various nanostructures, such as nanowires, nanobelts and nanosheets, of different semiconductors in a Chemical Vapor Deposition (CVD) system.

In the first part of my research, I selected chalcogenides (such as CdS and CdSe) for a comprehensive study in growing two-segment axial nanowires and radial nanobelts/sheets using the ternary CdSxSe1-x alloys. I demonstrated simultaneous red (from CdSe-rich) and green (from CdS-rich) light emission from a single monolithic heterostructure with a maximum wavelength separation of 160 nm. I also demonstrated the first simultaneous two-color lasing from a single nanosheet heterostructure with a wavelength separation of 91 nm under sufficiently strong pumping power.

In the second part, I considered several combinations of source materials with different growth methods in order to extend the spectral coverage of previously demonstrated structures towards shorter wavelengths to achieve full-color emissions. I achieved this with the growth of multisegment heterostructure nanosheets (MSHNs), using ZnS and CdSe chalcogenides, via our novel growth method. By utilizing this method, I demonstrated the first growth of ZnCdSSe MSHNs with an overall lattice mismatch of 6.6%, emitting red, green and blue light simultaneously, in a single furnace run using a simple CVD system. The key to this growth method is the dual ion exchange process which converts nanosheets rich in CdSe to nanosheets rich in ZnS, demonstrated for the first time in this work. Tri-chromatic white light emission with different correlated color temperature values was achieved under different growth conditions. We demonstrated multicolor (191 nm total wavelength separation) laser from a single monolithic semiconductor nanostructure for the first time. Due to the difficulties associated with growing semiconductor materials of differing composition on a given substrate using traditional planar epitaxial technology, our nanostructures and growth method are very promising for various device applications, including but not limited to: illumination, multicolor displays, photodetectors, spectrometers and monolithic multicolor lasers.

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Date Created
  • 2015

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Growth of novel semiconducting nano and heterostructures

Description

This dissertation presents research findings on the three materials systems: lateral Si nanowires (SiNW), In2Se3/Bi2Se3 heterostructures and graphene. The first part of the thesis was focused on the growth and

This dissertation presents research findings on the three materials systems: lateral Si nanowires (SiNW), In2Se3/Bi2Se3 heterostructures and graphene. The first part of the thesis was focused on the growth and characterization of lateral SiNW. Lateral here refers to wires growing along the plane of substrate; vertical NW on the other hand grow out of the plane of substrate. It was found, using the Au-seeded vapor – liquid – solid technique, that epitaxial single-crystal SiNW can be grown laterally along Si(111) substrates that have been miscut toward [11− 2]. The ratio of lateral-to-vertical NW was found to increase as the miscut angle increased and as disilane pressure and substrate temperature decreased. Based on this observation, growth parameters were identified whereby all of the deposited Au seeds formed lateral NW. Furthermore, the nanofaceted substrate guided the growth via a mechanism that involved pinning of the trijunction at the liquid/solid interface of the growing nanowire.

Next, the growth of selenide heterostructures was explored. Specifically, molecular beam epitaxy was utilized to grow In2Se3 and Bi2Se3 films on h-BN, highly oriented pyrolytic graphite and Si(111) substrates. Growth optimizations of In2Se3 and Bi2Se3 films were carried out by systematically varying the growth parameters. While the growth of these films was demonstrated on h-BN and HOPG surface, the majority of the effort was focused on growth on Si(111). Atomically flat terraces that extended laterally for several hundred nm, which were separated by single quintuple layer high steps characterized surface of the best In2Se3 films grown on Si(111). These In2Se3 films were suitable for subsequent high quality epitaxy of Bi2Se3 .

The last part of this dissertation was focused on a recently initiated and ongoing study of graphene growth on liquid metal surfaces. The initial part of the study comprised a successful modification of an existing growth system to accommodate graphene synthesis and process development for reproducible graphene growth. Graphene was grown on Cu, Au and AuCu alloys at varioua conditions. Preliminary results showed triangular features on the liquid part of the Cu metal surface. For Au, and AuCu alloys, hexagonal features were noticed both on the solid and liquid parts.

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Date Created
  • 2014

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Nano-engineering metamaterials and metafilms for high-efficiency solar energy harvesting and conversion

Description

The energy crisis in the past decades has greatly boosted the search for alternatives to traditional fossil foils, and solar energy stands out as an important candidate due to its

The energy crisis in the past decades has greatly boosted the search for alternatives to traditional fossil foils, and solar energy stands out as an important candidate due to its cleanness and abundance. However, the relatively low conversion efficiency and energy density strongly hinder the utilization of solar energy in wider applications. This thesis focuses on employing metamaterials and metafilms to enhance the conversion efficiency of solar thermal, solar thermophotovoltaic (STPV) and photovoltaic systems.

A selective metamaterial solar absorber is designed in this thesis to maximize the absorbed solar energy and minimize heat dissipation through thermal radiation. The theoretically designed metamaterial solar absorber exhibits absorptance higher than 95% in the solar spectrum but shows emittance less than 4% in the IR regime. This metamaterial solar absorber is further experimentally fabricated and optically characterized. Moreover, a metafilm selective absorber with stability up to 600oC is introduced, which exhibits solar absorptance higher than 90% and IR emittance less than 10%.

Solar thermophotovoltaic energy conversion enhanced by metamaterial absorbers and emitters is theoretically investigated in this thesis. The STPV system employing selective metamaterial absorber and emitter is investigated in this work, showing its conversion efficiency between 8% and 10% with concentration factor varying between 20 and 200. This conversion efficiency is remarkably enhanced compared with the conversion efficiency for STPV system employing black surfaces (<2.5%).

Moreover, plasmonic light trapping in ultra-thin solar cells employing concave grating nanostructures is discussed in this thesis. The plasmonic light trapping inside an ultrathin GaAs layer in the film-coupled metamaterial structure is numerically demonstrated. By exciting plasmonic resonances inside this structure, the short-circuit current density for the film-coupled metamaterial solar cell is three times the short-circuit current for a free-standing GaAs layer.

The dissertation is concluded by discussing about the future work on selective solar thermal absorbers, STPV/TPV systems and light trapping structures. Possibilities to design and fabricate solar thermal absorber with better thermal stability will be discussed, the experimental work of TPV system will be conducted, and the light trapping in organic and perovskite solar cells will be looked into.

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Created

Date Created
  • 2016