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University of Notre Dame

1. Lu Zhang. Manipulation of the DNA and Colloids in Suspension and at Surfaces</h1>.

Degree: PhD, Chemical Engineering, 2009, University of Notre Dame

This thesis explores the manipulation of DNA and colloids in suspension and at surfaces. Specifically: (1) we investigate the evaporative self-assembly of DNA and colloidal particles at surfaces; (2) we explore the like-charge attraction between DNA and colloids in suspension; (3) we examine Janus particles with varied surface chemistry and inner structures as model systems to understand dielectrophoresis (DEP) of anisotropic particles. In chapter 2, we investigate multiple-ring formation from an evaporating DNA droplet, and demonstrate that an internal stagnation flow is responsible for the formation of precursor ring and repeated stick-slip motion leads to multiple-ring formation. We further examine DNA-colloid binary suspensions as model systems to understand evaporation-induced interfacial hydrodynamics and self-assembled morphology of multi-component systems. The results demonstrate the feasibility of fabricating periodic self-assembled hybrid structures via one-step evaporation of droplets consisting of multiple components. In chapter 3, we investigate like-charge interaction of ÌøåÂ-DNA and colloids in aqueous suspension and the resultant DNA-colloid complex structures. Direct microscopic observations demonstrate enhanced adsorption of DNA on like-charge colloids with the addition of monovalent or divalent salts. Zeta potential measurements indicate that functionalized colloids remain negatively charged with increasing ionic strength, suggesting that screened electrostatic repulsion can account for enhanced DNA adsorption in high ionic strength media, despite the possible hydrophobic origin for DNA adsorption in low ionic strength media. Additionally, DNA-mediated colloid clustering is observed and the optimal DNA and salt concentration ranges are explored to predict the formation of considerable fractions of DNA-induced colloidal doublets, which could lead to a simple and rapid method to synthesize colloidal clusters of desirable shape and bio-functionality. In chapter 4, we examine Janus particles as model systems to understand dielectrophoresis of anisotropic particles. Janus particles with gold-coated hemisphere or with assembled COOH-end thiol monolayer on gold-capped hemisphere always experience positive DEP. Janus particles with assembled CH3-end thiol monolayer on gold-capped hemisphere exhibit negative DEP to positive DEP (n-to-p) crossover frequencies at high medium conductivities because interfacial polarization dominates at low frequencies and conductive gold layer dominates at high frequencies. Advisors/Committee Members: Yingxi Elaine Zhu, Committee Member, Marya Lieberman, Committee Member, Paul Bohn, Committee Member, Marvin Miller, Committee Chair, Hsueh-Chia Chang, Committee Member.

Subjects/Keywords: Janus particles; dielectrophoresis; colloids; DNA; self-assembly; like-charge attraction

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APA · Chicago · MLA · Vancouver · CSE | Export to Zotero / EndNote / Reference Manager

APA (6th Edition):

Zhang, L. (2009). Manipulation of the DNA and Colloids in Suspension and at Surfaces</h1>. (Doctoral Dissertation). University of Notre Dame. Retrieved from https://curate.nd.edu/show/gt54kk93p16

Chicago Manual of Style (16th Edition):

Zhang, Lu. “Manipulation of the DNA and Colloids in Suspension and at Surfaces</h1>.” 2009. Doctoral Dissertation, University of Notre Dame. Accessed June 26, 2019. https://curate.nd.edu/show/gt54kk93p16.

MLA Handbook (7th Edition):

Zhang, Lu. “Manipulation of the DNA and Colloids in Suspension and at Surfaces</h1>.” 2009. Web. 26 Jun 2019.

Vancouver:

Zhang L. Manipulation of the DNA and Colloids in Suspension and at Surfaces</h1>. [Internet] [Doctoral dissertation]. University of Notre Dame; 2009. [cited 2019 Jun 26]. Available from: https://curate.nd.edu/show/gt54kk93p16.

Council of Science Editors:

Zhang L. Manipulation of the DNA and Colloids in Suspension and at Surfaces</h1>. [Doctoral Dissertation]. University of Notre Dame; 2009. Available from: https://curate.nd.edu/show/gt54kk93p16

2. Li, Dong. Self-assembly Behaviors of Macroions in Dilute Solution.

Degree: PhD, Chemistry, 2012, Lehigh University

Subjects/Keywords: Hepatitis B virus; Like charge attraction; Macroion; Nanocage; Polyoxometalates; Self-assembly; Chemistry; Physical Sciences and Mathematics

…important attraction of like-charged bio-macroions. Counterion condensation around DNA macroions… …x29; described in the chapter. Their surface charge densities are listed in Table 1… …The concentration of {Mo72V30} is 0.026 mM. Bottom: Charge density on {… …54 Figure 3.3 Average Rh of vesicle-like structures in 0.20 mg/mL nanocage aqueous… …for the large vesicle-like structures self-assembled from M12L24 nanocages in diluted DMSO… 

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APA · Chicago · MLA · Vancouver · CSE | Export to Zotero / EndNote / Reference Manager

APA (6th Edition):

Li, D. (2012). Self-assembly Behaviors of Macroions in Dilute Solution. (Doctoral Dissertation). Lehigh University. Retrieved from https://preserve.lehigh.edu/etd/1308

Chicago Manual of Style (16th Edition):

Li, Dong. “Self-assembly Behaviors of Macroions in Dilute Solution.” 2012. Doctoral Dissertation, Lehigh University. Accessed June 26, 2019. https://preserve.lehigh.edu/etd/1308.

MLA Handbook (7th Edition):

Li, Dong. “Self-assembly Behaviors of Macroions in Dilute Solution.” 2012. Web. 26 Jun 2019.

Vancouver:

Li D. Self-assembly Behaviors of Macroions in Dilute Solution. [Internet] [Doctoral dissertation]. Lehigh University; 2012. [cited 2019 Jun 26]. Available from: https://preserve.lehigh.edu/etd/1308.

Council of Science Editors:

Li D. Self-assembly Behaviors of Macroions in Dilute Solution. [Doctoral Dissertation]. Lehigh University; 2012. Available from: https://preserve.lehigh.edu/etd/1308

3. Sinkovits, Daniel. Electrostatically-driven self-assembly of polyelectrolytes and colloidal tetrapods.

Degree: PhD, 0240, 2013, University of Illinois – Urbana-Champaign

I present research in the aggregation and self-assembly of charged macromolecules. This work aligns along three themes. The first theme is the effective interactions and aggregation of rodlike polyelectrolytes. The second theme is the self-assembly of colloidal tetrapods using Monte Carlo simulation. The third theme is the new techniques that needed to be devised in order to perform this work. Chapter 2 presents an extensive exploration of the free-energy landscapes governing the interaction between two rodlike polyelectrolytes with additional trivalent salt. Analysis reveals the relative stability of different aggregated configurations and the likely pathways taken toward first contact and subsequent rearrangement. Chapter 3 presents a study of the effect of including the low dielectric constant interior of rodlike polyelectrolytes has on their mutual interactions, paying particular attention to the many-body interactions, making connection to the stability of a hexagonal-packed bundle. I also explain the mechanism of interaction using ion distributions and pair correlation functions. Finally, I investigate quantitatively to what extent the effect of polarizability is simply to create an additional soft excluded-volume potential. In Chapter 4, I present study of the self-assembly of charge-functionalize colloidal tetrapods that have full mobility using Monte Carlo simulation. I find a change in the degree and structure of aggregation with increasing coupling. I also study the addition of positively or negatively charged nanoparticles, demonstrating a concentration-dependent change in the aggregate structure. Chapter 5 presents a new Monte Carlo simulation algorithm that was used to perform the work in Chapter 4. It is an extension of the geometric cluster algorithm that allows the simulation of anisotropic particles. I provide a detailed derivation of the algorithm, and I also include benchmark results and a study of the efficiency of the algorithm compared to Metropolis Monte Carlo. Chapter 6 explains the correct method for pressure calculation in systems that contain dielectric objects, as was the case for the periodic hexagonal array of polarizable polyelectrolytes simulated in Chapter 3. I also present a review of pressure calculation with periodic boundary conditions, since this is relevant to the dielectric calculation and there fundamental subtleties that are not treated in textbooks nor do concise reviews exist in the literature. Advisors/Committee Members: Luijten, Erik (advisor), Ceperley, David M. (Committee Chair), Luijten, Erik (committee member), Wong, Gerard C.L. (committee member), Gollin, George D. (committee member).

Subjects/Keywords: electrostatics; self-assembly; Monte Carlo; free energy; dielectric; polarization; like-charge attraction; cluster algorithm; rod; tetrapod; hypersphere; quaternion

like-charge attraction and many-body interactions. These effects are largely due to the fact… …it were the only ion present. Like-charge attraction is important because it allows many… …continuously moving ions. Entropy is highly relevant. Chapters 2 and 3 both study like-charge… …attraction, which refers to a phenomenon in which two highly charged macroions of the same sign… …counterions in the solution are multivalent, that is, having more than one electron charge. Unlike… 

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APA · Chicago · MLA · Vancouver · CSE | Export to Zotero / EndNote / Reference Manager

APA (6th Edition):

Sinkovits, D. (2013). Electrostatically-driven self-assembly of polyelectrolytes and colloidal tetrapods. (Doctoral Dissertation). University of Illinois – Urbana-Champaign. Retrieved from http://hdl.handle.net/2142/42215

Chicago Manual of Style (16th Edition):

Sinkovits, Daniel. “Electrostatically-driven self-assembly of polyelectrolytes and colloidal tetrapods.” 2013. Doctoral Dissertation, University of Illinois – Urbana-Champaign. Accessed June 26, 2019. http://hdl.handle.net/2142/42215.

MLA Handbook (7th Edition):

Sinkovits, Daniel. “Electrostatically-driven self-assembly of polyelectrolytes and colloidal tetrapods.” 2013. Web. 26 Jun 2019.

Vancouver:

Sinkovits D. Electrostatically-driven self-assembly of polyelectrolytes and colloidal tetrapods. [Internet] [Doctoral dissertation]. University of Illinois – Urbana-Champaign; 2013. [cited 2019 Jun 26]. Available from: http://hdl.handle.net/2142/42215.

Council of Science Editors:

Sinkovits D. Electrostatically-driven self-assembly of polyelectrolytes and colloidal tetrapods. [Doctoral Dissertation]. University of Illinois – Urbana-Champaign; 2013. Available from: http://hdl.handle.net/2142/42215

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