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1.
Clarke, Kimberly C.
The fabrication and study of stimuli-responsive microgel-based modular assemblies.
Degree: PhD, Chemistry and Biochemistry, 2015, Georgia Tech
URL: http://hdl.handle.net/1853/53918 
► This dissertation describes the development of temperature and pH-responsive interfaces, where the emphasis is placed on tuning the responsivities within a physiological temperature range. This…
(more)
▼ This dissertation describes the development of temperature and pH-responsive interfaces, where the emphasis is placed on tuning the responsivities within a physiological temperature range. This tuning is achieved through the utilization of polymeric building blocks, where each component is specifically synthesized to have a unique responsivity. The assembly of these components onto surfaces permits the fabrication of stimuli-responsive interfaces. In addition, this dissertation explores the use of a self-assembling peptide as a modular building block to modify the interface of hydrogel microparticles, resulting in the formation of a new biosynthetic construct.
Hydrogels are three-dimensional, crosslinked polymer networks that swell in water. Over the years, hydrogels have been extensively explored as biomaterials due to their high water content, tunable mechanics, and chemical versatility. Two areas where hydrogels have received considerable interest are drug delivery and extracellular matrices. Unfortunately, developing structurally and functionally complex hydrogels from the top down is challenging because many parameters cannot be independently tuned in a bulk material. An alternative route would be to develop a library of building blocks, where each is tailored for a given function, and assemble these components into composite structures. The building block synthesized and utilized in this dissertation is a microgel. Microgels are a colloidal dispersion of hydrogel microparticles, ranging in size from 100 to 1000 nm in diameter. The microgels were prepared from environmentally responsive polymers, sensitive to both temperature and pH.
Microgels have been used in the fabrication of polyelectrolyte layer-by-layer films, where the microgel serves as the polyanion and a linear polycation is used to “stitch” the particles together. In Chapters 3 and 4, stimuli-responsive interfaces are prepared from environmentally responsive microgel building blocks. In particular, Chapter 3 demonstrates tuning of the film response temperature by preparing several different microgels with differing ratios of two thermoresponsive polymers. Chapter 4 evaluates the influence of the pH environment on the thermoresponsivity of microgel films. While the pH environment was found to substantially affect some films, it is possible to prepare microgel films that behave independently of pH. The swelling/de-swelling of the films was also investigated by atomic force microscopy (AFM) as a function of both pH and temperature. It was determined that the AFM imaging parameters can drastically affect the measured film thicknesses (Appendix A) due to the soft, deformable nature of microgel films. The studies in these chapters illustrate the advantages of preparing composite structures from discrete components, where the functionality of the composite is dictated by the constituent particles.
In Chapter 5, attention is placed on modifying the surface of microgel particles. Many of the traditional routes used to modify microgels involve the…
Advisors/Committee Members: Lyon, L. Andrew (advisor), Fernández, Facundo M. (committee member), Hud, Nick (committee member), Collard, David (committee member), Sulchek, Todd (committee member).
Subjects/Keywords: Responsive interfaces; Surface modification; Microgel; Nanoparticles; Stimuli-responsive; Self-assembling peptide; Atomic force microscopy
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APA (6th Edition):
Clarke, K. C. (2015). The fabrication and study of stimuli-responsive microgel-based modular assemblies. (Doctoral Dissertation). Georgia Tech. Retrieved from http://hdl.handle.net/1853/53918
Chicago Manual of Style (16th Edition):
Clarke, Kimberly C. “The fabrication and study of stimuli-responsive microgel-based modular assemblies.” 2015. Doctoral Dissertation, Georgia Tech. Accessed October 19, 2019.
http://hdl.handle.net/1853/53918.
MLA Handbook (7th Edition):
Clarke, Kimberly C. “The fabrication and study of stimuli-responsive microgel-based modular assemblies.” 2015. Web. 19 Oct 2019.
Vancouver:
Clarke KC. The fabrication and study of stimuli-responsive microgel-based modular assemblies. [Internet] [Doctoral dissertation]. Georgia Tech; 2015. [cited 2019 Oct 19].
Available from: http://hdl.handle.net/1853/53918.
Council of Science Editors:
Clarke KC. The fabrication and study of stimuli-responsive microgel-based modular assemblies. [Doctoral Dissertation]. Georgia Tech; 2015. Available from: http://hdl.handle.net/1853/53918
2.
Hansen, Caroline Elizabeth.
A platelet-mediated paradigm for the targeted delivery of microencapsulated, clot-augmenting biotherapeutics.
Degree: PhD, Chemistry and Biochemistry, 2017, Georgia Tech
URL: http://hdl.handle.net/1853/58716
► Reported herein is a paradigm-shifting, targeted drug delivery system that leverages the patient’s own platelets to sense and actuate targeted delivery of a clot-augmenting therapeutic…
(more)
▼ Reported herein is a paradigm-shifting, targeted drug delivery system that leverages the patient’s own platelets to sense and actuate targeted delivery of a clot-augmenting therapeutic to a site of vascular injury. In this system, platelets target microencapsulated drugs through their natural aggregation behavior in the clot formation process and then deliver the drug by physically rupturing the microcapsule through contractile forces exerted during clot contraction. This cell-mediated, targeted drug delivery system utilizes polyelectrolyte multilayer capsules that hybridize with the patient’s own platelets upon intravenous administration and rupture upon platelet contraction, enabling the targeted and controlled “burst” release of an encapsulated biotherapeutics. As platelets are the “first responders” in the blood clot formation process, this platelet-hybridized system is ideal for the targeted delivery of clot augmenting biotherapeutics wherein immediate therapeutic efficacy is required. As proof-of-concept, we tailored this system to deliver the pro-clotting biotherapeutic, factor VIII (fVIII) for hemophilia A patients who have developed inhibitory anti-fVIII antibodies. The polyelectrolyte multilayer capsules physically shield the encapsulated fVIII from the patient’s inhibitors during circulation, preserving its bioactivity until it is delivered at the target site via platelet contractile force. Using an in vitro microfluidic vascular injury model with fVIII-inhibited blood, we demonstrate a 3.8x increase in induced fibrin formation using capsules loaded with fVIII at a concentration an order of magnitude lower than that used in systemic delivery. We further demonstrate that clot formation occurs 18 minutes faster when fVIII loaded capsules are used compared to systemic delivery at the same concentration. Because platelets are integral in the pathophysiology of thrombotic disorders, cancer, and innate immunity, this paradigm-shifting smart drug delivery system can be similarly applied to these diseases.
Advisors/Committee Members: Oyelere, Adegboyega (advisor), Lam, Wilbur A. (committee member), Lyon, L. Andrew (committee member), France, Stefan (committee member), Finn, M. G. (committee member).
Subjects/Keywords: Targeted drug delivery; Platelet contraction
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APA (6th Edition):
Hansen, C. E. (2017). A platelet-mediated paradigm for the targeted delivery of microencapsulated, clot-augmenting biotherapeutics. (Doctoral Dissertation). Georgia Tech. Retrieved from http://hdl.handle.net/1853/58716
Chicago Manual of Style (16th Edition):
Hansen, Caroline Elizabeth. “A platelet-mediated paradigm for the targeted delivery of microencapsulated, clot-augmenting biotherapeutics.” 2017. Doctoral Dissertation, Georgia Tech. Accessed October 19, 2019.
http://hdl.handle.net/1853/58716.
MLA Handbook (7th Edition):
Hansen, Caroline Elizabeth. “A platelet-mediated paradigm for the targeted delivery of microencapsulated, clot-augmenting biotherapeutics.” 2017. Web. 19 Oct 2019.
Vancouver:
Hansen CE. A platelet-mediated paradigm for the targeted delivery of microencapsulated, clot-augmenting biotherapeutics. [Internet] [Doctoral dissertation]. Georgia Tech; 2017. [cited 2019 Oct 19].
Available from: http://hdl.handle.net/1853/58716.
Council of Science Editors:
Hansen CE. A platelet-mediated paradigm for the targeted delivery of microencapsulated, clot-augmenting biotherapeutics. [Doctoral Dissertation]. Georgia Tech; 2017. Available from: http://hdl.handle.net/1853/58716
3.
Kodlekere, Purva Ganesh.
Development of multifunctional microgels for novel biomedical applications.
Degree: PhD, Chemistry and Biochemistry, 2015, Georgia Tech
URL: http://hdl.handle.net/1853/54439
► A range of microgels with two different functionalities were synthesized, and their utility in novel bioapplications was examined. Cationic microgels with varying properties were developed…
(more)
▼ A range of microgels with two different functionalities were synthesized, and their utility in novel bioapplications was examined. Cationic microgels with varying properties were developed by tuning synthesis conditions. Their size and primary amine content was analyzed, and one microgel system was selected as a model construct. Its primary amine groups were conjugated to two dyes with properties favorable for utilization as contrast agents in photoacoustic imaging. The concentration of contrast agent in single particles was determined. The implications of a high local dye concentration in the generation of high intensity photoacoustic signals, are discussed. The second bioapplication involved the targeted delivery of fibrinolytics to fibrin clots, in order to bring about dissolution of abnormal thrombi. For this purpose, core/shell microgels with carboxylic acid groups in their shells were synthesized in three size ranges. Following this, their dimension based differential localization in and around porous fibrin clots was examined. Fibrin-specific peptides were then conjugated onto the shells of these particles and the conjugates were shown to demonstrate strong interactions with the fibrin clots. The microgels conjugated to the peptide with the highest binding affinity to fibrin, were observed to bring about disruption of fibrin clots, merely through interference in the dynamic interactions among clot fibers, due to the equilibrium nature of the fibrin polymer. The implications of these novel results and future studies required to facilitate a better understanding of the phenomena involved, are discussed.
Advisors/Committee Members: Lyon, L. Andrew (advisor), Finn, M. G. (committee member), Dickson, Robert (committee member), Fernández, Facundo M. (committee member), Santangelo, Philip (committee member), Champion, Julie (committee member).
Subjects/Keywords: Microgels; Microgel characterization; Functional microgels; Microgel bioapplications; Cationic microgels; Bioconjugation; Dye conjugation; Photoacoustic imaging; Targeted delivery; Fibrin; Perfusion studies; Fibrinolytics; Core/shell microgels; Dynamic light scattering; Colloids
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APA (6th Edition):
Kodlekere, P. G. (2015). Development of multifunctional microgels for novel biomedical applications. (Doctoral Dissertation). Georgia Tech. Retrieved from http://hdl.handle.net/1853/54439
Chicago Manual of Style (16th Edition):
Kodlekere, Purva Ganesh. “Development of multifunctional microgels for novel biomedical applications.” 2015. Doctoral Dissertation, Georgia Tech. Accessed October 19, 2019.
http://hdl.handle.net/1853/54439.
MLA Handbook (7th Edition):
Kodlekere, Purva Ganesh. “Development of multifunctional microgels for novel biomedical applications.” 2015. Web. 19 Oct 2019.
Vancouver:
Kodlekere PG. Development of multifunctional microgels for novel biomedical applications. [Internet] [Doctoral dissertation]. Georgia Tech; 2015. [cited 2019 Oct 19].
Available from: http://hdl.handle.net/1853/54439.
Council of Science Editors:
Kodlekere PG. Development of multifunctional microgels for novel biomedical applications. [Doctoral Dissertation]. Georgia Tech; 2015. Available from: http://hdl.handle.net/1853/54439
4.
Dreaden, Erik Christopher.
Chemistry, photophysics, and biomedical applications of gold nanotechnologies.
Degree: PhD, Chemistry and Biochemistry, 2012, Georgia Tech
URL: http://hdl.handle.net/1853/51320
► Gold nanoparticles exhibit a combination of physical, chemical, optical, and electronic properties unique from all other nanotechnologies. These structures can provide a highly multifunctional platform…
(more)
▼ Gold nanoparticles exhibit a combination of physical, chemical, optical, and electronic properties unique from all other nanotechnologies. These structures can provide a highly multifunctional platform with which to diagnose and treat diseases and can dramatically enhance a variety of photonic and electronic processes and devices. The work herein highlights some newly emerging applications of these phenomena as they relate to the targeted diagnosis and treatment of cancer, improved charge carrier generation in photovoltaic device materials, and strategies for enhanced spectrochemical analysis and detection. Chapter 1 introduces the reader to the design, synthesis, and molecular functionalization of gold nanotechnologies, and provides a framework from which to discuss the unique photophysical properties and applications of these nanoscale materials and their physiological interactions in Chapter 2. Chapter 3 discusses ongoing preclinical research in our lab investigating the use of near-infrared absorbing gold nanorods as photothermal contrast agents for laser ablation therapy of solid tumors. In Chapter 4, we present recent work developing a novel strategy for the targeted treatment of hormone-dependent breast and prostate tumors using multivalent gold nanoparticles that function as highly selective and potent endocrine receptor antagonist chemotherapeutics. In Chapter 5, we discuss a newly-emerging tumor-targeting strategy for nanoscale drug carriers which relies on their selective delivery to immune cells that exhibit high accumulation and infiltration into breast and brain tumors. Using this platform, we further investigate the interactions of nanoscale drug carriers and imaging agents to a transmembrane protein considered to be the single most prevalent and single most important
contributor to drug resistance and the failure of chemotherapy. Chapter 6 presents work from a series of studies exploring enhanced charge carrier generation and relaxation in a hybrid electronic system exhibiting resonant interactions between photovoltaic device materials and plasmonic gold nanoparticles. Chapter 7 concludes by presenting studies investigating the contributions from so-called “dark” plasmon modes to the spectrochemical diagnostic method known as surface enhanced Raman scattering.
Advisors/Committee Members: El-Sayed, Mostafa A. (advisor), Oyelere, Adegboyega K. (committee member), Barry, Bridgette A. (committee member), Lyon, L. Andrew (committee member), Wang, Zhong Lin (committee member).
Subjects/Keywords: Multidrug resistance; Exciton; Semiconductor; Computational electrodynamics; Lithography; Antiestrogen; Colloid chemistry; Pharmacokinetics; Pharmaceuticals; Plasmon resonance; Macrophage; Spectroscopy; Hormone therapy; GPRC6A; Bioconjugation; Photothermal therapy; Laser; Pharmacodynamics; SPR; Nanoscience; Ultrafast; Antiandrogen; Plasmonics; SERS; Nanomedicine; Drug delivery; EPR; Au; Nanoparticles; Nanomedicine; Cancer; Gold
…and Prof. C.K. Payne (Georgia Tech). B) Photoacoustic
cytometry/tomography…
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APA (6th Edition):
Dreaden, E. C. (2012). Chemistry, photophysics, and biomedical applications of gold nanotechnologies. (Doctoral Dissertation). Georgia Tech. Retrieved from http://hdl.handle.net/1853/51320
Chicago Manual of Style (16th Edition):
Dreaden, Erik Christopher. “Chemistry, photophysics, and biomedical applications of gold nanotechnologies.” 2012. Doctoral Dissertation, Georgia Tech. Accessed October 19, 2019.
http://hdl.handle.net/1853/51320.
MLA Handbook (7th Edition):
Dreaden, Erik Christopher. “Chemistry, photophysics, and biomedical applications of gold nanotechnologies.” 2012. Web. 19 Oct 2019.
Vancouver:
Dreaden EC. Chemistry, photophysics, and biomedical applications of gold nanotechnologies. [Internet] [Doctoral dissertation]. Georgia Tech; 2012. [cited 2019 Oct 19].
Available from: http://hdl.handle.net/1853/51320.
Council of Science Editors:
Dreaden EC. Chemistry, photophysics, and biomedical applications of gold nanotechnologies. [Doctoral Dissertation]. Georgia Tech; 2012. Available from: http://hdl.handle.net/1853/51320
5.
Herman, Emily Sue.
Exploring complex interactions within microgels and microgel assemblies.
Degree: PhD, Chemistry and Biochemistry, 2014, Georgia Tech
URL: http://hdl.handle.net/1853/52998
► Hydrogels are water-swellable cross-linked polymeric networks that are capable of incorporating a variety of functionalities and responsivities. The stable colloidal form of a hydrogel is…
(more)
▼ Hydrogels are water-swellable cross-linked polymeric networks that are capable of incorporating a variety of functionalities and responsivities. The stable colloidal form of a hydrogel is known as a microgel and ranges in size from the nano- to the micrometer scale. Microgels can exhibit similar properties to hydrogels, but the colloidal size of the microgel creates differences in their responsive behavior, such as faster reaction kinetics, as compared to their macrogel counterpart. Microgels have been explored for a broad range of applications, either as individual entities or within large scale assemblies. Although these materials have shown a great deal of utility and versatility, microgels have also demonstrated a great deal of complexity due to the fact that they exhibit both polymeric and colloidal properties. This so-called polymer/colloid duality creates intricacies in characterizing the behavior of these materials, especially when coupled with an oppositely charged component within multilayered assemblies. In this dissertation, work is focused primarily on building a greater fundamental understanding of microgels and their behavior within large scale assemblies. This is done through the development of new characterization techniques or through a direct visualization of the interactions of microgels with their surrounding environment with emphasis on their interaction with an oppositely charged linear polyelectrolyte. From these studies, a more developed fundamental understanding of microgels and their assembly into complex structures is obtained, and these findings will aide in the development of future applications of microgel assemblies.
Advisors/Committee Members: Lyon, L. Andrew (advisor), Bottomley, Lawrence A. (committee member), Dickson, Robert (committee member), Fernandez-Nieves, Alberto (committee member), Hernandez, Rigoberto (committee member).
Subjects/Keywords: Microgel; Hydrogel; Polyelectrolyte; Film assembly; Colloids
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APA (6th Edition):
Herman, E. S. (2014). Exploring complex interactions within microgels and microgel assemblies. (Doctoral Dissertation). Georgia Tech. Retrieved from http://hdl.handle.net/1853/52998
Chicago Manual of Style (16th Edition):
Herman, Emily Sue. “Exploring complex interactions within microgels and microgel assemblies.” 2014. Doctoral Dissertation, Georgia Tech. Accessed October 19, 2019.
http://hdl.handle.net/1853/52998.
MLA Handbook (7th Edition):
Herman, Emily Sue. “Exploring complex interactions within microgels and microgel assemblies.” 2014. Web. 19 Oct 2019.
Vancouver:
Herman ES. Exploring complex interactions within microgels and microgel assemblies. [Internet] [Doctoral dissertation]. Georgia Tech; 2014. [cited 2019 Oct 19].
Available from: http://hdl.handle.net/1853/52998.
Council of Science Editors:
Herman ES. Exploring complex interactions within microgels and microgel assemblies. [Doctoral Dissertation]. Georgia Tech; 2014. Available from: http://hdl.handle.net/1853/52998
6.
Smith, Aubrey L.
Facilitating multi-electron reactivity at low-coordinate cobalt complexes using redox-active ligands.
Degree: PhD, Chemistry and Biochemistry, 2011, Georgia Tech
URL: http://hdl.handle.net/1853/42745
► In this study, we describe a detailed investigation of cobalt complexes containing redox-active ligands. We have prepared an electronic series of the complex in three…
(more)
▼ In this study, we describe a detailed investigation of cobalt complexes containing redox-active ligands. We have prepared an electronic series of the complex in three oxidation states: [CoIII(ap)2]-, CoIII(isq)(ap), and [CoIII(CH3CN)(isq)2]+. Characterization shows that the metal center remains cobalt(III) through the redox changes and indicates that the oxidation state changes occur with gain or loss of electrons from the ligand set. While CoIII(isq)(ap) reacts with halide radicals to form a new cobalt-halide bond in a single electron reaction, [CoIII(ap)2]- appears to be prone to multi-electron reactivity in reactions with sources of "Cl+". Both reactions occur with electrons derived from the ligand set. Mechanistic studies suggest a single, two electron step is responsible for the bond-formation. Similarly, [CoIII(ap)2]- reacts with alkyl halides to pseudo-oxidatively add the alkyl at the cobalt center. The product of the reaction can be isolated and fully characterized and was found to be best assigned as CoIII(alkyl)(isq)2. This assignment indicates that the reaction occurs, again, with the new bond formed with two electrons formally derived from the ligand set and with no change in oxidation state at the metal center. Mechanistic investigations of the pseudo-oxidative addition suggest the reaction is SN2-like. The reaction occurs with a wide scope of alkyl halides, including those containing beta-hydrogens.
The cross-coupling reaction of CoIII(alkyl)(isq)2 with RZnX forms a new carbon-carbon bond. Similarly, the two electron oxidized complex [CoIII(CH3CN)(isq)2]+ reacts with organozinc reagents to couple two carbon nucleophiles and form a new carbon-carbon bond. Both reactions are successful with both sp2 and sp3 carbons. When followed substoichiometrically, the homocoupling reaction can be observed to form CoIII(alkyl)(isq)2. This indicates that the homocoupling and cross-coupling reactions proceed by the same mechanism. However, both reactions have low yields. The yield of the reactions are decreased by steric bulk of the alkyl or aryl fragments or around the metal center created by substituents on the ligand. Also, while the steric congestion disfavors the addition of the first alkyl fragment, the addition of the second alkyl fragment and subsequent rapid elimination of the coupling product is almost completely inhibited. This result also implies that the coupling of the two alkyl fragments is entirely inner-sphere requiring installation of both for coupling.
In a complementary study, use of bidentate or tridentate stabilizing ligands in combination with one redox-active catechol-derived or amidophenol-derived ligand was investigated. With the synthesis of (triphos)CoII(cat) and the one electron oxidized [(triphos)CoII(sq)]+, it is evident that the oxidation occurs at the ligand and not the metal. Reaction of (triphos)CoII(cat) with a Cl+ reagent generated a new material which we tentatively describe as (triphos)CoIII(Cl)(sq). This implies that the two electrons used to create the new cobalt-halide bond…
Advisors/Committee Members: Soper, Jake D. (Committee Chair), Barefield, E. Kent (Committee Member), Jones, Christopher W. (Committee Member), Lyon, L. Andrew (Committee Member), Zhang, Z. John (Committee Member).
Subjects/Keywords: Coupling; Carbon-carbon; Redox-active ligand; Catalysis; Cobalt; Oxidation; Chemical reactions; Charge exchange; Ligands (Biochemistry)
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APA (6th Edition):
Smith, A. L. (2011). Facilitating multi-electron reactivity at low-coordinate cobalt complexes using redox-active ligands. (Doctoral Dissertation). Georgia Tech. Retrieved from http://hdl.handle.net/1853/42745
Chicago Manual of Style (16th Edition):
Smith, Aubrey L. “Facilitating multi-electron reactivity at low-coordinate cobalt complexes using redox-active ligands.” 2011. Doctoral Dissertation, Georgia Tech. Accessed October 19, 2019.
http://hdl.handle.net/1853/42745.
MLA Handbook (7th Edition):
Smith, Aubrey L. “Facilitating multi-electron reactivity at low-coordinate cobalt complexes using redox-active ligands.” 2011. Web. 19 Oct 2019.
Vancouver:
Smith AL. Facilitating multi-electron reactivity at low-coordinate cobalt complexes using redox-active ligands. [Internet] [Doctoral dissertation]. Georgia Tech; 2011. [cited 2019 Oct 19].
Available from: http://hdl.handle.net/1853/42745.
Council of Science Editors:
Smith AL. Facilitating multi-electron reactivity at low-coordinate cobalt complexes using redox-active ligands. [Doctoral Dissertation]. Georgia Tech; 2011. Available from: http://hdl.handle.net/1853/42745
7.
Whitmire, Rachel Elisabeth.
Self-assembling polymeric nanoparticles for enhanced intra-articular anti-inflammatory protein delivery.
Degree: PhD, Mechanical Engineering, 2012, Georgia Tech
URL: http://hdl.handle.net/1853/43587
► The goal of this thesis was to develop a new drug-delivering material to deliver anti-inflammatory protein for treating OA. Our central hypothesis for this work…
(more)
▼ The goal of this thesis was to develop a new drug-delivering material to deliver anti-inflammatory protein for treating OA. Our central hypothesis for this work is that a controlled release/presentation system will more effectively deliver anti-inflammatory protein therapies to the OA joint.
The primary goal of this work was to synthesize a block copolymer that could self-assemble into injectable, sub-micron-scale particles and would allow an anti-inflammatory protein, IL-1ra, to be tethered to its surface for efficient protein delivery. The block copolymer incorporated an oligo-ethylene monomer for tissue compatibility and non-fouling behavior, a 4-nitrophenol group for efficient protein tethering, and cyclohexyl methacrylate, a hydrophobic monomer, for particle stability. We engineered the copolymer and tested it in both in vitro culture experiments and an in vivo model to evaluate protein retention in the knee joint. The rationale for this project was that the rational design and synthesis of a new drug- and protein-delivering material can create a modular polymer particle that can deliver multi-faceted therapies to treat OA.
This work characterizes the in vitro and in vivo behavior of our polymer particle system. The protein tethering strategy allows IL-1ra protein to be tethered to the surface of these particles. Once tethered, IL-1ra maintains its bioactivity and actively targets synoviocytes, cells crucial to the OA pathology. This binding happens in an IL-1-dependent manner. Furthermore, IL-1ra-tethered particles are able to inhibit IL-1beta-induced NF-kappaB activation. These studies show that this particle system has the potential to deliver IL-1ra to arthritic joints and that it has potential for localizing/targeting drugs to inflammatory cells of interest as a new way to target OA drug treatments.
Advisors/Committee Members: Garcia, Andres. J. (Committee Chair), Babensee, Julia (Committee Member), Levenston, Marc (Committee Member), Lyon, L. Andrew (Committee Member), McCarty, Nael (Committee Member), Murthy, Niren (Committee Member).
Subjects/Keywords: IL-1ra; Rats; Biomaterials; Osteoarthritis; Polymeric drug delivery system; Nanoparticles; Self-assembly (Chemistry); Osteoarthritis; Anti-inflammatory agents
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APA (6th Edition):
Whitmire, R. E. (2012). Self-assembling polymeric nanoparticles for enhanced intra-articular anti-inflammatory protein delivery. (Doctoral Dissertation). Georgia Tech. Retrieved from http://hdl.handle.net/1853/43587
Chicago Manual of Style (16th Edition):
Whitmire, Rachel Elisabeth. “Self-assembling polymeric nanoparticles for enhanced intra-articular anti-inflammatory protein delivery.” 2012. Doctoral Dissertation, Georgia Tech. Accessed October 19, 2019.
http://hdl.handle.net/1853/43587.
MLA Handbook (7th Edition):
Whitmire, Rachel Elisabeth. “Self-assembling polymeric nanoparticles for enhanced intra-articular anti-inflammatory protein delivery.” 2012. Web. 19 Oct 2019.
Vancouver:
Whitmire RE. Self-assembling polymeric nanoparticles for enhanced intra-articular anti-inflammatory protein delivery. [Internet] [Doctoral dissertation]. Georgia Tech; 2012. [cited 2019 Oct 19].
Available from: http://hdl.handle.net/1853/43587.
Council of Science Editors:
Whitmire RE. Self-assembling polymeric nanoparticles for enhanced intra-articular anti-inflammatory protein delivery. [Doctoral Dissertation]. Georgia Tech; 2012. Available from: http://hdl.handle.net/1853/43587
8.
Hendrickson, Grant R.
Harnessing microgel softness for biointerfacing.
Degree: PhD, Chemistry and Biochemistry, 2013, Georgia Tech
URL: http://hdl.handle.net/1853/50252
► Hydrogel materials have become a heavily studied as materials for interfacing with biology both for laboratory investigations and the development of devices for biomedical applications.…
(more)
▼ Hydrogel materials have become a heavily studied as materials for interfacing with biology both for laboratory investigations and the development of devices for biomedical applications. These polymers are water swellable and can be made responsive to many different stimuli by choice of monomers, co-monomers, and cross-linkers or functionalization with pendent ligands, substrates, or charged groups. The high water content, low moduli and potential responsively of these polymers make good candidates for biomaterials. A specific type of hydrogel called a microgel or a hydrogel micro/nanoparticle has similar properties to bulk hydrogel materials. Many of the interesting results and utility of the microgels in bioapplications are due to their inherent softness of the material. Here, the softness, flexibility, and conformability of these water swollen particles is used to create an interesting sensor platform, studied in the context of a microgel passing through a pore, and used as an emulsifier to create a drug delivery platform. The unifying theme of this dissertation is the softness of microgels which is critical for all of these experiments. However, the study of individual microgel softness is challenging and complex, since the softness is composed of two different components. The first is that the microgel is a swollen polymer which can be deswollen by an external stimuli or force. The second is that the microgel is a volume conserving elastic colloid which can deform without deswelling under the certain conditions. Throughout, this dissertation will discuss the ramifications of the complex softness of microgels in each experimental result and potential application.
Advisors/Committee Members: Lyon, L. Andrew (advisor), Perry, Joseph W. (committee member), Dickson, Robert M. (committee member), Janata, Jiri (committee member), Wartell, Roger M. (committee member), Lyon, Louis A. (committee member).
Subjects/Keywords: Microgel; Hydrogel; Biomaterial; Polymer physics; Biological interfaces; Colloids
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APA (6th Edition):
Hendrickson, G. R. (2013). Harnessing microgel softness for biointerfacing. (Doctoral Dissertation). Georgia Tech. Retrieved from http://hdl.handle.net/1853/50252
Chicago Manual of Style (16th Edition):
Hendrickson, Grant R. “Harnessing microgel softness for biointerfacing.” 2013. Doctoral Dissertation, Georgia Tech. Accessed October 19, 2019.
http://hdl.handle.net/1853/50252.
MLA Handbook (7th Edition):
Hendrickson, Grant R. “Harnessing microgel softness for biointerfacing.” 2013. Web. 19 Oct 2019.
Vancouver:
Hendrickson GR. Harnessing microgel softness for biointerfacing. [Internet] [Doctoral dissertation]. Georgia Tech; 2013. [cited 2019 Oct 19].
Available from: http://hdl.handle.net/1853/50252.
Council of Science Editors:
Hendrickson GR. Harnessing microgel softness for biointerfacing. [Doctoral Dissertation]. Georgia Tech; 2013. Available from: http://hdl.handle.net/1853/50252
9.
Yang, Si Kyung.
Orthogonal functionalization strategies in polymeric materials.
Degree: PhD, Chemistry and Biochemistry, 2009, Georgia Tech
URL: http://hdl.handle.net/1853/31684
► This thesis describes original research aimed at the development of highly efficient polymer functionalization strategies by introducing orthogonal chemistry within polymeric systems. The primary hypothesis…
(more)
▼ This thesis describes original research aimed at the development of highly efficient polymer functionalization strategies by introducing orthogonal chemistry within polymeric systems. The primary hypothesis of this thesis is that the use of click chemistries or noncovalent interactions can provide new and easy pathways towards the synthesis of highly functionalized polymers thereby addressing the shortcomings of traditional covalent functionalization approaches. To verify the hypothesis, the work presented in the following chapters of this thesis further explores previous methods of either covalent or noncovalent polymer functionalization described in Chapter 1.
Chapters 2 and 3 present advanced methods of covalent polymer functionalization based on high-yielding and orthogonal click reactions: 1,3-dipolar cycloaddition, hydrazone formation, and maleimide-thiol coupling. All three click reactions employed can be orthogonal to one another and conversions can be quantitative, leading to the easy and rapid synthesis of highly functionalized polymers without interference among functional handles along the polymer backbones.
The next two chapters focus on the noncovalent functionalization strategies for creating supramolecular block copolymers via the main-chain self-assembly of telechelic polymers. Novel synthetic methods to prepare telechelic polymers bearing terminal recognition motifs were developed through a combination of ROMP using functionalized ruthenium initiators and functionalized chain-terminators, and the resulting polymers were self-assembled to form supramolecular block copolymers. Chapter 4 demonstrates the formation of supramolecular multiblock copolymers via self-assembly of symmetrical telechelic polymers using metal coordination, while Chapter 5 demonstrates that supramolecular ABC triblock copolymers can be prepared by the self-assembly of a heterotelechelic polymer as the central block with two other complementary monotelechelic polymers using two orthogonal hydrogen bonding interactions.
Chapter 6 presents a unique application of noncovalent functionalization approaches. The ultimate goal of this research is to develop a controlled polymerization method based on noncovalent templation. The initial attempts at the metal coordination-based template polymerization are presented in this chapter.
Finally, Chapter 7 summarizes the findings in each chapter and presents the potential extensions of the orthogonal functionalization strategies developed in this thesis.
Advisors/Committee Members: Weck, Marcus (Committee Chair), Breedveld, Victor (Committee Member), Fahrni, Christoph (Committee Member), Kelly, Wendy (Committee Member), Lyon, L. Andrew (Committee Member).
Subjects/Keywords: Supramolecular interactions; Click chemistry; Orthogonal functionalization; Olefin metathesis; Polymers; Copolymers; Polymerization; Ring-opening polymerization; Hydrogen bonding; Functions, Orthogonal
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APA (6th Edition):
Yang, S. K. (2009). Orthogonal functionalization strategies in polymeric materials. (Doctoral Dissertation). Georgia Tech. Retrieved from http://hdl.handle.net/1853/31684
Chicago Manual of Style (16th Edition):
Yang, Si Kyung. “Orthogonal functionalization strategies in polymeric materials.” 2009. Doctoral Dissertation, Georgia Tech. Accessed October 19, 2019.
http://hdl.handle.net/1853/31684.
MLA Handbook (7th Edition):
Yang, Si Kyung. “Orthogonal functionalization strategies in polymeric materials.” 2009. Web. 19 Oct 2019.
Vancouver:
Yang SK. Orthogonal functionalization strategies in polymeric materials. [Internet] [Doctoral dissertation]. Georgia Tech; 2009. [cited 2019 Oct 19].
Available from: http://hdl.handle.net/1853/31684.
Council of Science Editors:
Yang SK. Orthogonal functionalization strategies in polymeric materials. [Doctoral Dissertation]. Georgia Tech; 2009. Available from: http://hdl.handle.net/1853/31684
10.
Blackburn, William H.
Microgel bioconjugates for targeted delivery to cancer cells.
Degree: PhD, Chemistry and Biochemistry, 2008, Georgia Tech
URL: http://hdl.handle.net/1853/31792
► The use of hydrogel nanoparticles, or nanogels, as targeted delivery vehicles to cancer cells was described. The nanogels were synthesized by free radical precipitation polymerization,…
(more)
▼ The use of hydrogel nanoparticles, or nanogels, as targeted delivery vehicles to cancer cells was described. The nanogels were synthesized by free radical precipitation polymerization, with poly(N-isopropylmethacrylamide) as the main monomer, and have a core/shell architecture. The nanogels were near 50 nm in radius, contained fluorescein for visualization, and had an amine-containing shell for bioconjugation, making these particles ideal for delivery studies. The nanogels were conjugated with the YSA (YSAYPDSVPMMSC) peptide, which is an ephrin mimic, allowing for uptake by the EphA2 (erythropoietin-producing hepatocellular) receptor. We have delivered YSA-conjugated nanogels to Hey cells and BG-1 cells, as evidenced by fluorescence microscopy. We have shown that the nanogels can encapsulate siGLO Red Transfection Indicator (siGLO) and deliver the siGLO to Hey cells in vitro. After successful delivery of the non-targeting siGLO, we delivered siRNA for knockdown of epidermal growth factor receptor (EGFR). We have shown protein knockdown from 24-120 h after nanogel delivery, as well as knockdown with different siRNA concentrations delivered to the cells. Furthermore, addition of taxol following EGFR knockdown suggests that the chemosensitivity of the Hey cells is increased. Successful in vitro delivery of the nanogels prompted in vivo studies with the nanogels. The nanogels were used to encapsulate silver nanoclusters for potential bioimaging applications. Targeting of the nanogels to MatrigelTM plugs in mice suggest that the particles hold promise as in vivo delivery agents.
Advisors/Committee Members: Lyon, L. Andrew (Committee Chair), Barry, Bridgette (Committee Member), Fahrni, Christoph J. (Committee Member), Hud, Nicholas V. (Committee Member), Le Doux, Joseph M. (Committee Member).
Subjects/Keywords: In vivo; In vitro; SiRNA; Nanogels; Targeted delivery; Colloids; Colloids in medicine; Drug delivery systems
…and Lyon, L. Andrew.
“Bioconjugation of Soft Nanomaterials”, Biomedical Nanostructures, John…
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APA (6th Edition):
Blackburn, W. H. (2008). Microgel bioconjugates for targeted delivery to cancer cells. (Doctoral Dissertation). Georgia Tech. Retrieved from http://hdl.handle.net/1853/31792
Chicago Manual of Style (16th Edition):
Blackburn, William H. “Microgel bioconjugates for targeted delivery to cancer cells.” 2008. Doctoral Dissertation, Georgia Tech. Accessed October 19, 2019.
http://hdl.handle.net/1853/31792.
MLA Handbook (7th Edition):
Blackburn, William H. “Microgel bioconjugates for targeted delivery to cancer cells.” 2008. Web. 19 Oct 2019.
Vancouver:
Blackburn WH. Microgel bioconjugates for targeted delivery to cancer cells. [Internet] [Doctoral dissertation]. Georgia Tech; 2008. [cited 2019 Oct 19].
Available from: http://hdl.handle.net/1853/31792.
Council of Science Editors:
Blackburn WH. Microgel bioconjugates for targeted delivery to cancer cells. [Doctoral Dissertation]. Georgia Tech; 2008. Available from: http://hdl.handle.net/1853/31792
11.
Li, Tai-De.
Atomic force microscopy study of nano-confined liquids.
Degree: PhD, Physics, 2008, Georgia Tech
URL: http://hdl.handle.net/1853/24674
► In this thesis, we investigate the structural and dynamical properties of nano-confined liquids by means of a new AFM-based technique that has the ability to…
(more)
▼ In this thesis, we investigate the structural and dynamical properties of nano-confined liquids by
means of a new AFM-based technique that has the ability to measure normal force, lateral force, and the distance between the AFM tip and the sample simultaneously. Thanks to the mechanical stability of our apparatus, a judicious choice, and a new mechanical drift analysis, we are able to measure the tip-sample distance with sub-angstrom resolution, all the way down to the last liquid layer.
Advisors/Committee Members: Riedo, Elisa (Committee Chair), Davidovic, Dragomir (Committee Member), Goldman, Daniel I. (Committee Member), Landman, Uzi (Committee Member), Lyon, L. Andrew (Committee Member).
Subjects/Keywords: AFM; Nano-confiend liquids; Tribology; Rheology; Nanoelectromechanical systems; Nanostructured materials; Fluid dynamics; Fluid mechanics
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APA (6th Edition):
Li, T. (2008). Atomic force microscopy study of nano-confined liquids. (Doctoral Dissertation). Georgia Tech. Retrieved from http://hdl.handle.net/1853/24674
Chicago Manual of Style (16th Edition):
Li, Tai-De. “Atomic force microscopy study of nano-confined liquids.” 2008. Doctoral Dissertation, Georgia Tech. Accessed October 19, 2019.
http://hdl.handle.net/1853/24674.
MLA Handbook (7th Edition):
Li, Tai-De. “Atomic force microscopy study of nano-confined liquids.” 2008. Web. 19 Oct 2019.
Vancouver:
Li T. Atomic force microscopy study of nano-confined liquids. [Internet] [Doctoral dissertation]. Georgia Tech; 2008. [cited 2019 Oct 19].
Available from: http://hdl.handle.net/1853/24674.
Council of Science Editors:
Li T. Atomic force microscopy study of nano-confined liquids. [Doctoral Dissertation]. Georgia Tech; 2008. Available from: http://hdl.handle.net/1853/24674
Georgia Tech
12.
Kim, Jongseong.
Stimuli-Responsive Hydrogel Microlenses.
Degree: PhD, Chemistry and Biochemistry, 2007, Georgia Tech
URL: http://hdl.handle.net/1853/14496
► This dissertation is aimed towards using stimuli-responsive pNIPAm-co-AAc microgels synthesized via free-radical precipitation polymerization to prepare stimuli-responsive hydrogel microlenses. Chapter 1 gives a detailed background…
(more)
▼ This dissertation is aimed towards using stimuli-responsive pNIPAm-co-AAc microgels synthesized via free-radical precipitation polymerization to prepare stimuli-responsive hydrogel microlenses. Chapter 1 gives a detailed background of hydrogels, and their applications using responsive hydrogels. Chapter 2 describes the use of colloidal hydrogel microparticles as microlens elements and the fabrication method to form the hydrogel microlens arrays via Coulombic interactions. Chapter 3 shows the demonstration of tunable microlenses prepared by the method used in Chapter 2. In this chapter the microlenses are subjected to various pH and temperature in aqueous solutions. Chapter 4 describes that the microlens arrays constructed on Au nanoparticle-functionalized glass substrates by self-assembly display dramatic changes in lensing power in response to an impingent frequency-doubled Nd:YAG laser. The microlens photoswitching is highly reversible, with sub-millisecond lens switching times. Chapter 5 describes the development of bioresponsive hydrogel microlenses as a new protein detection technology. The microlens method is shown to be very specific for the target protein, with no detectable interference from nonspecific protein binding. Chapter 6 describes the use of bioresponsive hydrogel microlenses as a label-free biosensing scaffolding. These microstructures simultaneously act as the biosensors scaffolding/immobilization architecture, transducer, amplifier, and also allow for broad tunability of the analyte concentration to which the microlens is sensitive.
Advisors/Committee Members: Lyon, L. Andrew (Committee Chair), Dickson, Robert (Committee Member), Janata, Jiri (Committee Member), Srinivasarao, Mohan (Committee Member), Weck, Marcus (Committee Member).
Subjects/Keywords: Biosensing; Bioresponsive Hydrogel; Responsive Hydrogel; Microlens; Hydrogel
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APA (6th Edition):
Kim, J. (2007). Stimuli-Responsive Hydrogel Microlenses. (Doctoral Dissertation). Georgia Tech. Retrieved from http://hdl.handle.net/1853/14496
Chicago Manual of Style (16th Edition):
Kim, Jongseong. “Stimuli-Responsive Hydrogel Microlenses.” 2007. Doctoral Dissertation, Georgia Tech. Accessed October 19, 2019.
http://hdl.handle.net/1853/14496.
MLA Handbook (7th Edition):
Kim, Jongseong. “Stimuli-Responsive Hydrogel Microlenses.” 2007. Web. 19 Oct 2019.
Vancouver:
Kim J. Stimuli-Responsive Hydrogel Microlenses. [Internet] [Doctoral dissertation]. Georgia Tech; 2007. [cited 2019 Oct 19].
Available from: http://hdl.handle.net/1853/14496.
Council of Science Editors:
Kim J. Stimuli-Responsive Hydrogel Microlenses. [Doctoral Dissertation]. Georgia Tech; 2007. Available from: http://hdl.handle.net/1853/14496
Georgia Tech
13.
Kim, Gloria J.
Cancer nanotechnology: engineering multifunctional nanostructures for targeting tumor cells and vasculatures.
Degree: PhD, Biomedical Engineering, 2007, Georgia Tech
URL: http://hdl.handle.net/1853/22610
► Significant progress has been made in the development of new agents against cancer and new ways of delivering existing and new agents. Yet, the major…
(more)
▼ Significant progress has been made in the development of new agents against cancer and new ways of delivering existing and new agents. Yet, the major challenge to target and selectively kill cancer cells while affecting as few healthy cells as possible remains. When linked with tumor targeting moieties such as tumor-specific ligands or monoclonal antibodies, nanoparticles can be used to target cancer-specific receptors, tumor biomarkers as well as tumor vasculatures with high affinity and precision. Recently, the use of nanoparticles for drug delivery and targeting has emerged as one of the most exciting and clinically important areas in cancer nanotechnology.
In this work, we tested the hypothesis that our novel ternary biomolecular nanostructures of folic acid (FA), biodegradable polymer, and paclitaxel will improve the delivery and tumor-specific distribution of the anticancer drug. The design was based on three principles: 1) Passive targeting via enhanced permeation and retention (EPR) effect; 2) active targeting via a tumor-specific ligand; and 3) prodrug that would release the drug upon delivery. First, self-assembled polymer-paclitaxel-FA nanostructures were synthesized. Their physicochemical properties were examined and biological efficacy was tested. The conjugates had significantly improved solubility in water, enabling cremophor-free formulation. Second, in vitro cellular toxicity and targeting ability of the nanostructures were investigated. In cancer cell lines with high folate receptor (FR) expression, the ternary conjugates were efficiently taken up whereas no detectable association was found in cells with minimal or no FR expression. Third, in vivo investigation in human xenograft mice models was carried out. Ternary nanostructures drastically inhibited tumor growth without inducing systemic toxicity or side effects. The ternary nanostructures displayed remarkable anti-angiogenic effect on tumor vasculature. Heparin-paclitaxel-FA was also very effective in drug resistant tumors, potentially overcoming multidrug resistance. Studies in other cancer models are in progress to determine the spectrum of applicability of these ternary nanostructures. The design principles applied in these nanoparticles can be extended to delivery and targeting of diagnostic and imaging agents. The ability to engineer multifunctional nanostructures will have a significant impact on cancer diagnostics, molecular profiling, and the integration of cancer therapy and imaging.
Advisors/Committee Members: Nie, Shuming (Committee Chair), Lyon, L. Andrew (Committee Member), McIntire, Larry V. (Committee Member), Murthy, Niren (Committee Member), Prausnitz, Mark R. (Committee Member).
Subjects/Keywords: Drug resistance; Cancer; Heparin; Drug delivery; Folate targeting; Nanotechnology; Nanoparticles; Cancer Treatment; Drug targeting
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APA (6th Edition):
Kim, G. J. (2007). Cancer nanotechnology: engineering multifunctional nanostructures for targeting tumor cells and vasculatures. (Doctoral Dissertation). Georgia Tech. Retrieved from http://hdl.handle.net/1853/22610
Chicago Manual of Style (16th Edition):
Kim, Gloria J. “Cancer nanotechnology: engineering multifunctional nanostructures for targeting tumor cells and vasculatures.” 2007. Doctoral Dissertation, Georgia Tech. Accessed October 19, 2019.
http://hdl.handle.net/1853/22610.
MLA Handbook (7th Edition):
Kim, Gloria J. “Cancer nanotechnology: engineering multifunctional nanostructures for targeting tumor cells and vasculatures.” 2007. Web. 19 Oct 2019.
Vancouver:
Kim GJ. Cancer nanotechnology: engineering multifunctional nanostructures for targeting tumor cells and vasculatures. [Internet] [Doctoral dissertation]. Georgia Tech; 2007. [cited 2019 Oct 19].
Available from: http://hdl.handle.net/1853/22610.
Council of Science Editors:
Kim GJ. Cancer nanotechnology: engineering multifunctional nanostructures for targeting tumor cells and vasculatures. [Doctoral Dissertation]. Georgia Tech; 2007. Available from: http://hdl.handle.net/1853/22610
Georgia Tech
14.
St. John, Ashlee Nicole.
Compression effects on the phase behavior of microgel assemblies.
Degree: PhD, Chemistry and Biochemistry, 2008, Georgia Tech
URL: http://hdl.handle.net/1853/22666
► Microgels are a class of colloids that are mechanically soft, and while in many cases can behave similarly to their hard-sphere counterparts, their interaction potentials…
(more)
▼ Microgels are a class of colloids that are mechanically soft, and while in many cases can behave similarly to their hard-sphere counterparts, their interaction potentials are quite different. The softness of the interaction between microgels makes them capable of deformation and compression into more concentrated assemblies. This concentrated regime is interesting because little, if any, experimental work has been done to see how the bulk properties of soft-sphere assemblies deviate from those of hard-spheres at the point where their interaction potentials begin to diverge. In this thesis the effects on assembly phase behavior and dynamics of both particle compression and softness of the interaction potential are addressed. Poly(N-isopropylacrylamide) (pNIPAm) microgels are an excellent model system in which to study these effects. The thermoresponsivity of the polymer provides the experimentalist with a dial to tune the volume fraction of an assembly, while maintaining a constant particle number density in the system. Optical microscopy, particle tracking analysis and rheology have been used to investigate the effects of packing and particle structure on equilibrium phase behavior and localized perturbations to the phase of the assembly of this soft-sphere system. It has been elucidated from these experiments and others involving deswelling of large microgel particles in the presence of high concentrations of smaller microgels, that the soft, repulsive interaction between microgels is caused by a longer-range repulsion than was previously believed. The particles are acting on each other from a distance through the osmotic pressure of the assembly, which causes each particle to deswell without coming into direct contact with a neighboring particle.
Advisors/Committee Members: Lyon, L. Andrew (Committee Chair), Breedveld, Victor (Committee Member), Hernandez, Rigoberto (Committee Member), Srininvasarao, Mohan (Committee Member), Weeks, Eric R. (Committee Member).
Subjects/Keywords: Phase behavior; Colloids; Poly(N-isopropylacrylamide); Microgels; Colloids; Nanoparticles; Materials – Compression testing
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APA (6th Edition):
St. John, A. N. (2008). Compression effects on the phase behavior of microgel assemblies. (Doctoral Dissertation). Georgia Tech. Retrieved from http://hdl.handle.net/1853/22666
Chicago Manual of Style (16th Edition):
St. John, Ashlee Nicole. “Compression effects on the phase behavior of microgel assemblies.” 2008. Doctoral Dissertation, Georgia Tech. Accessed October 19, 2019.
http://hdl.handle.net/1853/22666.
MLA Handbook (7th Edition):
St. John, Ashlee Nicole. “Compression effects on the phase behavior of microgel assemblies.” 2008. Web. 19 Oct 2019.
Vancouver:
St. John AN. Compression effects on the phase behavior of microgel assemblies. [Internet] [Doctoral dissertation]. Georgia Tech; 2008. [cited 2019 Oct 19].
Available from: http://hdl.handle.net/1853/22666.
Council of Science Editors:
St. John AN. Compression effects on the phase behavior of microgel assemblies. [Doctoral Dissertation]. Georgia Tech; 2008. Available from: http://hdl.handle.net/1853/22666
Georgia Tech
15.
Serpe, Michael Joseph.
Self-Assembly of Poly(N-isopropylacrylamide) Microgel Thin Films.
Degree: PhD, Chemistry and Biochemistry, 2004, Georgia Tech
URL: http://hdl.handle.net/1853/4806
► The assembly of poly(N-isopropylacrylamide-co-acrylic acid) (pNIPAm-co-AAc) microgel thin films into disordered and ordered arrays was investigated. Disordered pNIPAm-co-AAc microgel arrays were assembled based on electrostatic…
(more)
▼ The assembly of poly(N-isopropylacrylamide-co-acrylic acid) (pNIPAm-co-AAc) microgel thin films into disordered and ordered arrays was investigated. Disordered pNIPAm-co-AAc microgel arrays were assembled based on electrostatic attractions between polyanionic pNIPAm-co-AAc microgels and polycationic poly(allylamine hydrochloride) (PAH). These interactions were studied in solution and subsequently used to assemble thin films following a Layer-by-Layer assembly protocol. Thin films were assembled as a function of pNIPAm-co-AAc microgel solution temperature and the resultant film thermoresponsivity characterized as a function of microgel layer number and pH. The response of assembled thin films to pH 3.0 and 6.5 exposure was then characterized by quartz crystal impedance and surface plasmon resonance spectroscopy, which showed that the thin film solvation was highly dependent on the pH of the solution it was in. Assembled thin films were also shown to be useful as controlled drug delivery platforms, where it was found that small molecules could be released from the films in a temperature regulated fashion. Microgel thin films also exhibited unique optical properties and were used as microlens arrays, which were able to focus pattern in air as well as in solution and had focal lengths that could be tuned in response to pH and temperature changes. Ordered microgel arrays were assembled following a thermal annealing process, in order to make light diffracting materials. These ordered arrays were photopolymerized and exhibited temperature dependent Bragg diffraction properties.
Advisors/Committee Members: Lyon, L. Andrew (Committee Chair), Janata, Jiri (Committee Member), Ludovice, Peter (Committee Member), Mizaikoff, Boris (Committee Member), Orlando, Thomas (Committee Member).
Subjects/Keywords: Quartz crystal impedance; Drug delivery; Microlens; Thermoresponsive; Multilayer; Layer-by-Layer; Hydrogel; Polymeric drug delivery systems; Thin films; Colloids Synthesis; Nanoparticles
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APA (6th Edition):
Serpe, M. J. (2004). Self-Assembly of Poly(N-isopropylacrylamide) Microgel Thin Films. (Doctoral Dissertation). Georgia Tech. Retrieved from http://hdl.handle.net/1853/4806
Chicago Manual of Style (16th Edition):
Serpe, Michael Joseph. “Self-Assembly of Poly(N-isopropylacrylamide) Microgel Thin Films.” 2004. Doctoral Dissertation, Georgia Tech. Accessed October 19, 2019.
http://hdl.handle.net/1853/4806.
MLA Handbook (7th Edition):
Serpe, Michael Joseph. “Self-Assembly of Poly(N-isopropylacrylamide) Microgel Thin Films.” 2004. Web. 19 Oct 2019.
Vancouver:
Serpe MJ. Self-Assembly of Poly(N-isopropylacrylamide) Microgel Thin Films. [Internet] [Doctoral dissertation]. Georgia Tech; 2004. [cited 2019 Oct 19].
Available from: http://hdl.handle.net/1853/4806.
Council of Science Editors:
Serpe MJ. Self-Assembly of Poly(N-isopropylacrylamide) Microgel Thin Films. [Doctoral Dissertation]. Georgia Tech; 2004. Available from: http://hdl.handle.net/1853/4806
Georgia Tech
16.
Cheng, Shing-Yi.
Development of a Tissue Engineered Pancreatic Substitute Based on Genetically Engineered Cells.
Degree: PhD, Chemical Engineering, 2005, Georgia Tech
URL: http://hdl.handle.net/1853/7160
► Genetically engineered cells have the potential to solve the cell availability problem in developing a pancreatic tissue substitute for the treatment of insulin-dependent diabetes (IDD).…
(more)
▼ Genetically engineered cells have the potential to solve the cell availability problem in developing a pancreatic tissue substitute for the treatment of insulin-dependent diabetes (IDD). These cells can be beta-cells genetically engineered so that they can be grown in culture, such as the betaTC3 and betaTC tet mouse insulinomas developed by Efrat et al; or, they can be non-beta cells genetically engineered to secrete insulin constitutively or under transcriptional regulation. The aim of this work was to thoroughly characterize and improve the secretion dynamics of pancreatic substitutes based on genetically engineered cells.
One issue involved with the continuous beta-cell lines is the remodeling of the cells inside an encapsulated cell system, which may affect the insulin secretion dynamics exhibited by the construct. To evaluate the effect of remodeling on the secretion properties of the construct, we used a single-pass perfusion system to characterize the insulin secretion dynamics of different alginate beads in response to step-ups and downs in glucose concentration. Results indicated that the secretion dynamics of beads indeed changed after long-term culture. On the other hand, data with a growth-regulated cell line, betaTC tet cells, showed that the secretion profile of beads can be retained if the cell growth is suppressed.
A major concern associated with genetically engineered cells of non-beta origin is that they generally exhibit sub-optimal insulin secretion characteristics relative to normal pancreatic islets. Instead of relying on molecular tools such as manipulating gene elements, our approach was to introduce a glucose-responsive material acting as a control barrier for insulin release from a device containing constitutively secreting cells. Proof-of-concept experiments were performed with a disk-shaped prototype based on recombinant HepG2 hepatomas or C2C12 myoblasts, which constitutively secreted insulin, and concanavalin A (con A)-based glucose-responsive material as the control barrier. Results demonstrated that the a hybrid pancreatic substitute consisting of constitutively secreting cells and glucose-responsive material has the potential to provide a more physiologic regulation of insulin release than the cells by themselves or in an inert material.
Advisors/Committee Members: Sambanis, Athanassios (Committee Chair), Chaikof, Elliot (Committee Member), Lyon, L. Andrew (Committee Member), Thule, Peter (Committee Member), Wick, Timothy (Committee Member).
Subjects/Keywords: Pancreatic substitute; Insulin secretion dynamics; Glucose-responsive; Genetically engineered cells
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APA (6th Edition):
Cheng, S. (2005). Development of a Tissue Engineered Pancreatic Substitute Based on Genetically Engineered Cells. (Doctoral Dissertation). Georgia Tech. Retrieved from http://hdl.handle.net/1853/7160
Chicago Manual of Style (16th Edition):
Cheng, Shing-Yi. “Development of a Tissue Engineered Pancreatic Substitute Based on Genetically Engineered Cells.” 2005. Doctoral Dissertation, Georgia Tech. Accessed October 19, 2019.
http://hdl.handle.net/1853/7160.
MLA Handbook (7th Edition):
Cheng, Shing-Yi. “Development of a Tissue Engineered Pancreatic Substitute Based on Genetically Engineered Cells.” 2005. Web. 19 Oct 2019.
Vancouver:
Cheng S. Development of a Tissue Engineered Pancreatic Substitute Based on Genetically Engineered Cells. [Internet] [Doctoral dissertation]. Georgia Tech; 2005. [cited 2019 Oct 19].
Available from: http://hdl.handle.net/1853/7160.
Council of Science Editors:
Cheng S. Development of a Tissue Engineered Pancreatic Substitute Based on Genetically Engineered Cells. [Doctoral Dissertation]. Georgia Tech; 2005. Available from: http://hdl.handle.net/1853/7160
Georgia Tech
17.
Kim, Philseok.
Surface modification of nanoparticles for polymer/ceramic nanocomposites and their applications.
Degree: PhD, Chemistry and Biochemistry, 2008, Georgia Tech
URL: http://hdl.handle.net/1853/31651
► Polymer/ceramic nanocomposites benefit by combining high permittivities (r) of metal oxide nanoparticles with high dielectric strength and excellent solution-processability of polymeric hosts. Simple mixing of…
(more)
▼ Polymer/ceramic nanocomposites benefit by combining high permittivities (r) of metal oxide nanoparticles with high dielectric strength and excellent solution-processability of polymeric hosts. Simple mixing of nanoparticles and polymer generally results in poor quality materials due mainly to the agglomeration of nanoparticles and poor miscibility of nanoparticles in host materials. Surface modification of metal oxide nanoparticles with phosphonic acid-based ligands was found to afford a robust surface modification and improve the processablity and the quality of nanocomposites. The use of phosphonic-acid modified barium titanate (BaTiO₃) nanoparticles in dielectric nanocomposites dramatically improved the stability of the nanoparticle dispersion and the quality of the nanocomposites. Surface modification of BaTiO₃ nanoparticles allowed high quality nanocomposite thin films in ferroelectric polymer hosts such as poly(vinylidene fluoride-co-hexafluoropropylene) with large volume fractions (up to 50 vol. %), which exhibited a remarkable combination of a high permittvity (35 at 1 kHz) and a high breakdown strength (210 V/µm) leading to a maximum energy storage density of 6.1 J/cm³. The effect of nanoparticle volume fractions on the dielectric properties of this nanocomposite system was investigated and compared with theoretical models. At high volume fraction of nanoparticles, the porosity of the nanocomposites was found to have important role in the dielectric performance. A combined effective medium theory and finite difference simulation was used to model the dielectric properties of high volume fraction dielectric nanocomposites with porosity. These results provide a guideline to optimize the volume fractions of nanoparticles for maximum energy density. Nanocomposites based on phosphonic acid-modified BaTiO₃ nanoparticles can also be used as printable high permittivity dielectrics in organic electronics. High volume fractions (up to 37 vol. %) of phosphonic acid-modified BaTiO₃ nanoparticles dispersed in cross-linked poly(4-vinylphenol) allowed solution-processable high permittivity thin films with a large capacitance density (~50 nF/cm²) and a low leakage current (10 8 A/cm²) suitable as a gate insulator in organic field-effect transistors (OFETs). Pentacene-based OFETs using these nanocomposites showed a low threshold voltage (< -2.0 V) and a large on/off current ratio (Ion/off 104 ~ 106) due to the high capacitance density and low leakage current of the gate insulator.
Advisors/Committee Members: Perry, Joseph W. (Committee Chair), Kippelen, Bernard (Committee Member), Lyon, L. Andrew (Committee Member), Marder, Seth R. (Committee Member), Whetten, Robert L. (Committee Member).
Subjects/Keywords: Barium titanate; Dielectric nanocomposite; Phosphonic acid; Surface modification; Energy storage; Ligands (Biochemistry); Dielectrics; Nanocomposites (Materials); Capacitors
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APA (6th Edition):
Kim, P. (2008). Surface modification of nanoparticles for polymer/ceramic nanocomposites and their applications. (Doctoral Dissertation). Georgia Tech. Retrieved from http://hdl.handle.net/1853/31651
Chicago Manual of Style (16th Edition):
Kim, Philseok. “Surface modification of nanoparticles for polymer/ceramic nanocomposites and their applications.” 2008. Doctoral Dissertation, Georgia Tech. Accessed October 19, 2019.
http://hdl.handle.net/1853/31651.
MLA Handbook (7th Edition):
Kim, Philseok. “Surface modification of nanoparticles for polymer/ceramic nanocomposites and their applications.” 2008. Web. 19 Oct 2019.
Vancouver:
Kim P. Surface modification of nanoparticles for polymer/ceramic nanocomposites and their applications. [Internet] [Doctoral dissertation]. Georgia Tech; 2008. [cited 2019 Oct 19].
Available from: http://hdl.handle.net/1853/31651.
Council of Science Editors:
Kim P. Surface modification of nanoparticles for polymer/ceramic nanocomposites and their applications. [Doctoral Dissertation]. Georgia Tech; 2008. Available from: http://hdl.handle.net/1853/31651
Georgia Tech
18.
Nolan, Christine Marie.
Microgel Based Materials for Controlled Macromolecule Delivery.
Degree: PhD, Chemistry and Biochemistry, 2005, Georgia Tech
URL: http://hdl.handle.net/1853/6874
► This dissertation focuses on utilization of poly(N-isopropylacylamide) (pNIPAm) based mirogels for regulated macromolecule drug delivery applications. There is particular emphasis on incorporation of stimuli responsive…
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▼ This dissertation focuses on utilization of poly(N-isopropylacylamide) (pNIPAm) based mirogels for regulated macromolecule drug delivery applications. There is particular emphasis on incorporation of stimuli responsive materials into multi-layer thin film constructs with the main goal being fabrication of highly functional materials with tunable release characteristics. Chapter 1 gives a broad overview of hydrogel and microgel materials focusing on fundamental properties of pNIPAm derived materials. Chapter 2 illustrates the progression of controlled macromolecule release from hydrogel and microgel materials and sets up the scope of this thesis work. Chapter 3 details studies on thermally modulated insulin release from microgel thin films where extended pulsatile release capabilities are shown. Chapters 4 and 5 focus on more fundamental synthesis and characterization studies of PEG and acrylic acid modified pNIPAm microgels that could ultimately lead to the design of protein loaded microgel films with tunable release characteristics. Chapter 6 illustrates fundamental macromolecule loading strategies, which could also prove useful in future protein drug delivery design using stimuli responsive networks. Chapter 7 concentrates on direct insulin release studies that probe the interaction between entrapped and freely diffusing protein and microgels. These model experiments could prove useful in design of tunable macromolecule drug release from functionally modified microgels and could aid in the tailored design of peptide-loaded microgel thin films. Chapter 8 discusses the future outlook of controlled macromolecule release from microgel based materials.
Advisors/Committee Members: Lyon, L. Andrew (Committee Chair), Beckham, Haskell (Committee Member), Bottomley, Lawrence (Committee Member), El-Sayed, Mostafa (Committee Member), Mizaikoff, Boris (Committee Member).
Subjects/Keywords: Delivery; Macromolecules; Microgel; Hydrogel; Macromolecules; Nanoparticles; Colloids; Drug delivery systems
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APA (6th Edition):
Nolan, C. M. (2005). Microgel Based Materials for Controlled Macromolecule Delivery. (Doctoral Dissertation). Georgia Tech. Retrieved from http://hdl.handle.net/1853/6874
Chicago Manual of Style (16th Edition):
Nolan, Christine Marie. “Microgel Based Materials for Controlled Macromolecule Delivery.” 2005. Doctoral Dissertation, Georgia Tech. Accessed October 19, 2019.
http://hdl.handle.net/1853/6874.
MLA Handbook (7th Edition):
Nolan, Christine Marie. “Microgel Based Materials for Controlled Macromolecule Delivery.” 2005. Web. 19 Oct 2019.
Vancouver:
Nolan CM. Microgel Based Materials for Controlled Macromolecule Delivery. [Internet] [Doctoral dissertation]. Georgia Tech; 2005. [cited 2019 Oct 19].
Available from: http://hdl.handle.net/1853/6874.
Council of Science Editors:
Nolan CM. Microgel Based Materials for Controlled Macromolecule Delivery. [Doctoral Dissertation]. Georgia Tech; 2005. Available from: http://hdl.handle.net/1853/6874
Georgia Tech
19.
Jain, Prashant K.
Plasmons in assembled metal nanostructures: radiative and nonradiative properties, near-field coupling and its universal scaling behavior.
Degree: PhD, Chemistry and Biochemistry, 2008, Georgia Tech
URL: http://hdl.handle.net/1853/28207
► Noble metal nanostructures possess unique properties including large near-field enhancement and strong light scattering and absorption due to their plasmon resonance - the collective coherent…
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▼ Noble metal nanostructures possess unique properties including large near-field enhancement and strong light scattering and absorption due to their plasmon resonance - the collective coherent oscillation of the metal free electrons in resonance with the electromagnetic field of light. The effect of nanostructure size, shape, composition, and environment on the plasmon resonance frequency and plasmonic enhancement is well known. In this thesis, we describe the effect of inter-particle coupling in assembled plasmonic nanostructures on their radiative and non-radiative properties. When metal nanoparticles assemble, plasmon oscillations of neighboring particles couple, resulting in a shift in the plasmon resonance frequency. Our investigation of plasmon coupling in gold nanorods shows that the coupling between the plasmons is "bonding" in nature when the plasmon oscillations are polarized along the inter-particle axis, whereas an "anti-bonding" interaction results when the polarization is perpendicular. We studied the distance-dependence of plasmon coupling using electrodynamic simulations and experimental plasmon resonances of lithographically fabricated gold nanoparticle pairs with systematically varying inter-particle separations. The strength of plasmon bonding, reflected by the fractional plasmon shift, decays near-exponentially with the inter-particle separation (in units of particle size) according to a universal trend independent of the nanoparticle size, shape, metal type, or medium. From the universal scaling model, we obtain a "plasmon ruler equation" which calculates (in good agreement with the experiments of Alivisatos and Liphardt) the inter-particle separation in a gold nanosphere pair from its plasmon resonance shift, making it applicable to the determination of inter-site distances in biological systems. Universal size-scaling is valid also in the metal nanoshell structure, a nanosphere trimer, and pairs of elongated nanoparticles, thus making it a generalized fundamental model, which is useful in optimizing plasmon coupling for achieving tunable plasmon resonances, enhanced plasmonic sensitivities, and large SERS cross-sections. Ultrafast laser pump-probe studies of non-radiative electronic relaxation in coupled metal nanospheres in aggregates and in gold nanospheres conjugated to thiol SAMs are also reported. We also show that the relative contribution of scattering (radiative) to absorption (non-radiative) part of the plasmon relaxation, respectively useful in optical and photothermal applications, can be increased by increasing the nanostructure size.
Advisors/Committee Members: El-Sayed, Mostafa A. (Committee Chair), Lyon, L. Andrew (Committee Member), Sherrill, C. David (Committee Member), Wang, Zhong Lin (Committee Member), Whetten, Robert L. (Committee Member).
Subjects/Keywords: Nanotechnology; Plasmon coupling; Assembly; Surface plasmon resonance; Metal nanoparticles; Nanorods; Plasmons (Physics); Nanostructured materials; Precious metals; Surface plasmon resonance
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APA ·
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MLA ·
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Export
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APA (6th Edition):
Jain, P. K. (2008). Plasmons in assembled metal nanostructures: radiative and nonradiative properties, near-field coupling and its universal scaling behavior. (Doctoral Dissertation). Georgia Tech. Retrieved from http://hdl.handle.net/1853/28207
Chicago Manual of Style (16th Edition):
Jain, Prashant K. “Plasmons in assembled metal nanostructures: radiative and nonradiative properties, near-field coupling and its universal scaling behavior.” 2008. Doctoral Dissertation, Georgia Tech. Accessed October 19, 2019.
http://hdl.handle.net/1853/28207.
MLA Handbook (7th Edition):
Jain, Prashant K. “Plasmons in assembled metal nanostructures: radiative and nonradiative properties, near-field coupling and its universal scaling behavior.” 2008. Web. 19 Oct 2019.
Vancouver:
Jain PK. Plasmons in assembled metal nanostructures: radiative and nonradiative properties, near-field coupling and its universal scaling behavior. [Internet] [Doctoral dissertation]. Georgia Tech; 2008. [cited 2019 Oct 19].
Available from: http://hdl.handle.net/1853/28207.
Council of Science Editors:
Jain PK. Plasmons in assembled metal nanostructures: radiative and nonradiative properties, near-field coupling and its universal scaling behavior. [Doctoral Dissertation]. Georgia Tech; 2008. Available from: http://hdl.handle.net/1853/28207
Georgia Tech
20.
Sorrell, Courtney Davis.
Fundamental studies of responsive microgel thin films at interfaces.
Degree: PhD, Chemistry and Biochemistry, 2008, Georgia Tech
URL: http://hdl.handle.net/1853/24679
► The research described covers fundamental studies of environmentally-responsive microgel-based thin films as a function of film architecture, microgel chemistry, film thickness, and environmental stimulus. Studies…
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▼ The research described covers fundamental studies of environmentally-responsive microgel-based thin films as a function of film architecture, microgel chemistry, film thickness, and environmental stimulus. Studies of multi-layer microgel thin films were conducted primarily using atomic force microscopy (AFM), quartz crystal microgravimetry (QCM), and surface plasmon resonance (SPR), each of which probed different aspects the film architecture as a function of pH of the environment around the film. Binary thin films were constructed by changing the ratios and composition of the microgels in solution to create multi-functional thin films for surface modification applications and were studied using AFM. The basic understanding of how these components create films at surfaces gives us insight into how the films perform and will allow for greater diversity without the guesswork. The morphology of films created from microgels with a degradable cross-linker was examined by AFM as a function of degradation of the particles structure. This thesis focuses mainly on very thin microgel films (<5 layers) studied using QCM, SPR, and AFM. Additional studies involving the characterization of semi-soft colloidal paint-on photonics are discussed in Appendix A.
Advisors/Committee Members: Lyon, L. Andrew (Committee Chair), Beckham, Haskell (Committee Member), Janata, Jiri (Committee Member), Pielak, Gary (Committee Member), Ragauskas, Arthur (Committee Member).
Subjects/Keywords: Responsive polymers; Hydrogels; Microgels; Thin films; Atomic force microscopy; Thin films; Colloids
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APA ·
Chicago ·
MLA ·
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Export
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APA (6th Edition):
Sorrell, C. D. (2008). Fundamental studies of responsive microgel thin films at interfaces. (Doctoral Dissertation). Georgia Tech. Retrieved from http://hdl.handle.net/1853/24679
Chicago Manual of Style (16th Edition):
Sorrell, Courtney Davis. “Fundamental studies of responsive microgel thin films at interfaces.” 2008. Doctoral Dissertation, Georgia Tech. Accessed October 19, 2019.
http://hdl.handle.net/1853/24679.
MLA Handbook (7th Edition):
Sorrell, Courtney Davis. “Fundamental studies of responsive microgel thin films at interfaces.” 2008. Web. 19 Oct 2019.
Vancouver:
Sorrell CD. Fundamental studies of responsive microgel thin films at interfaces. [Internet] [Doctoral dissertation]. Georgia Tech; 2008. [cited 2019 Oct 19].
Available from: http://hdl.handle.net/1853/24679.
Council of Science Editors:
Sorrell CD. Fundamental studies of responsive microgel thin films at interfaces. [Doctoral Dissertation]. Georgia Tech; 2008. Available from: http://hdl.handle.net/1853/24679
. 
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