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You searched for +publisher:"University of Notre Dame" +contributor:("Bradley D. Smith, Research Director"). Showing records 1 – 2 of 2 total matches.

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University of Notre Dame

1. Kasey J Clear. Molecular Probes for Biomembrane Recognition.

Degree: PhD, Chemistry and Biochemistry, 2016, University of Notre Dame

The biological membrane is made up of primarily polar lipids and integral membrane proteins. Polar lipids are a broad class of amphiphilic biomolecules that serve diverse biological roles encompassing energy storage, cell compartmentalization, and cell signaling. The first part of the dissertation is an introduction to the structures of polar lipids and their self-assembly properties followed by a summary of biological strategies for polar lipid recognition. The final section of the first chapter is an introduction to synthetic receptors for polar lipids. The next two chapters focus on research towards new probes for anionic phospholipids such as phosphatidylserine (PS) using synthetic zinc(II)-bis(dipicolylamine) (Zn2BDPA) coordination complexes. PS targeting is relevant to cell death since PS is exposed on the surface of dead and dying cells. Zn2BDPA coordination complexes are known to selectively recognize PS-rich membranes and act as cell death molecular imaging agents. However, there is a need to improve in vivo imaging performance by selectively increasing target affinity and decreasing off-target accumulation. The first study (Chapter 2) focuses on the synthesis and screening of a small library of modified Zn2BDPA complexes constructed through the oxime ligation to better understand the structural requirements for membrane PS recognition. The second study (Chapter 3) compares the cell death targeting ability of two new phenoxide-bridged Zn2BDPA deep-red fluorescent probes in cells and two animal models of cell death. An [111]In-labelled radiotracer version of the monovalent probe also exhibited selective cell death targeting with the most favorable in vivo biodistribution profile yet reported for a Zn2BDPA complex. Thus, the monovalent phenoxide-bridged Zn2BDPA scaffold is a promising candidate for further development as a cell death imaging agent in living subjects. In chapters 4 and 5, the focus moves from developing affinity ligands for anionic lipid recognition to developing molecular design principles for liposomal pH nanosensors (Chapter 5) and new analytical strategies for anion detection using indicator displacement assays (Chapter 6). Advisors/Committee Members: Bradley D. Smith, Research Director, Robert Stahelin, Committee Member, Richard Taylor, Committee Member.

Subjects/Keywords: molecular recognition; anion recognition; cell death; organic chemistry; molecular imaging; lipids; fluorescence

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

APA (6th Edition):

Clear, K. J. (2016). Molecular Probes for Biomembrane Recognition. (Doctoral Dissertation). University of Notre Dame. Retrieved from https://curate.nd.edu/show/dv13zs2842v

Chicago Manual of Style (16th Edition):

Clear, Kasey J. “Molecular Probes for Biomembrane Recognition.” 2016. Doctoral Dissertation, University of Notre Dame. Accessed November 17, 2017. https://curate.nd.edu/show/dv13zs2842v.

MLA Handbook (7th Edition):

Clear, Kasey J. “Molecular Probes for Biomembrane Recognition.” 2016. Web. 17 Nov 2017.

Vancouver:

Clear KJ. Molecular Probes for Biomembrane Recognition. [Internet] [Doctoral dissertation]. University of Notre Dame; 2016. [cited 2017 Nov 17]. Available from: https://curate.nd.edu/show/dv13zs2842v.

Council of Science Editors:

Clear KJ. Molecular Probes for Biomembrane Recognition. [Doctoral Dissertation]. University of Notre Dame; 2016. Available from: https://curate.nd.edu/show/dv13zs2842v


University of Notre Dame

2. Evan M. Peck. Self-Assembly and Molecular Recognition Using Squaraine Rotaxanes.

Degree: PhD, Chemistry and Biochemistry, 2016, University of Notre Dame

Molecular recognition is ubiquitous within nature and controls nearly every aspect of organism structure and function. The ability of biological systems to spontaneously assemble has captured the imaginations of supramolecular chemists and has inspired elegant synthetic mimics that are diverse in both structure and function. The power and versatility offered by molecular recognition and self-assembly is rapidly expanding, and many synthetic receptors have now advanced beyond fundamental studies and are being pursued for practical applications. This thesis begins with an overview of molecular recognition, the underlying principles that control the phenomenon, and how chemists attempt to design host-guest systems based on this understanding. Of particular importance is the molecular recognition of organic dyes, as the majority of this thesis will focus on the molecular recognition and encapsulation of squaraine dyes to form stable structures known as squaraine rotaxanes (SRs). The thesis will then transition into the development of a new class of chromophores, thiosquaraine rotaxanes, and their evaluation as potential photodynamic therapy agents. The thesis next introduces SR endoperoxides (SREPs), storable SR analogues that emit light as they cleanly release singlet oxygen. A major drawback to current SREP systems is their very low chemiluminescence yield, and Chapter 3 discusses attempts to increase the light output using various chemical additives. The addition of these additives also led to the discovery and investigation of a new mechanism for light generation in SREPs. The last two chapters of the thesis focus on the development of a high affinity host-guest system that self-assembles in aqueous media. This system, termed Synthavidin (synthetic avidin) Technology, provides a new paradigm for molecular probe design. Chapter 4 focuses on the discovery of Synthavidin Technology, and the early stage development that led to a highly fluorescent squaraine-macrocycle system that self-assembles in water. Finally, Chapter 5 describes the use of a targeted Synthavidin probe as a bone imaging agent in small animal models. The Synthavidin probes are remarkably stable and demonstrate strong multivalent targeting of skeletal tissue. The thesis concludes with a look toward the future of Synthavidin Technology and its potential use in biomedical and therapeutic applications. Advisors/Committee Members: Bradley D. Smith, Research Director, Haifeng Gao, Committee Member, Olaf Wiest, Committee Member.

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

APA (6th Edition):

Peck, E. M. (2016). Self-Assembly and Molecular Recognition Using Squaraine Rotaxanes. (Doctoral Dissertation). University of Notre Dame. Retrieved from https://curate.nd.edu/show/hd76rx93c8f

Chicago Manual of Style (16th Edition):

Peck, Evan M.. “Self-Assembly and Molecular Recognition Using Squaraine Rotaxanes.” 2016. Doctoral Dissertation, University of Notre Dame. Accessed November 17, 2017. https://curate.nd.edu/show/hd76rx93c8f.

MLA Handbook (7th Edition):

Peck, Evan M.. “Self-Assembly and Molecular Recognition Using Squaraine Rotaxanes.” 2016. Web. 17 Nov 2017.

Vancouver:

Peck EM. Self-Assembly and Molecular Recognition Using Squaraine Rotaxanes. [Internet] [Doctoral dissertation]. University of Notre Dame; 2016. [cited 2017 Nov 17]. Available from: https://curate.nd.edu/show/hd76rx93c8f.

Council of Science Editors:

Peck EM. Self-Assembly and Molecular Recognition Using Squaraine Rotaxanes. [Doctoral Dissertation]. University of Notre Dame; 2016. Available from: https://curate.nd.edu/show/hd76rx93c8f

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