This thesis focuses on the development of new methods of single molecule spectroscopy for chemistry. The design, synthesis, and implementation of a novel optical tweezers platform forms the core of this work. Synthesized polystyrene@SiO2 core-shell beads exhibited stable trapping in a variety of organic solvents ranging in polarity and refractive index. Optical trapping had previously never been observed in many of these solvents. Atom-transfer radical polymerization and copper-free click chemistry were utilized to form single molecule tethers of poly(methyl methacrylate) in situ, and characterized with force-extension measurements. These experiments represent the first single molecule polymer tether formations using optical tweezers in a solvent other than water. This is the first widely solvent compatible optical tweezers platform.
A new method for performing force-detected spectroscopy using optical tweezers is also presented. This method of detection was applicable on a range of molecules, including quantum dots, a small molecule dye, and a protein chromophore. The sensitivity of this force-detected absorption technique is already in the 10s-100s of molecules, and a clear path forward exists to push this detection limit to the single molecule level. These new methods provide a foundation to conduct future single molecule experiments on a variety of organic and organometallic entities using techniques that were previously inaccessible to many chemists. With the versatility of the new platforms we hope single molecule spectroscopy using optical tweezers will become an even more powerful tool for chemical investigation.
|Commitee:||Ganim, Ziad, Hazari, Nilay, Miller, Scott|
|School Location:||United States -- Connecticut|
|Source:||DAI-B 81/3(E), Dissertation Abstracts International|
|Subjects:||Chemistry, Physical chemistry, Polymer chemistry|
|Keywords:||Atom transfer radical polymerization, Click chemistry, Force-detected absorption spectroscopy, Optical tweezers, Single molecule, Single molecule spectroscopy|
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