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Schorr.30 Dissertation.pdf (5.61 MB)

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Characterization of rare events in flow using surface enhanced Raman spectroscopy (SERS)

Schorr, Hannah C
http://orcid.org/0009-0000-1836-6893105
http://rave.ohiolink.edu/etdc/view?acc_num=osu1721175705847462

Abstract Details

2024, Doctor of Philosophy, Ohio State University, Chemistry.
Detecting, quantifying, and identifying flowing samples is imperative to many applications including pharmaceutical development and manufacturing, diagnostics, forensics, and environmental studies. Surface enhanced Raman spectroscopy (SERS) is a nondestructive, water insensitive, and highly sensitive method that can be applied to these areas. Raman spectroscopy provides information regarding molecular bonds based on the inelastic scattering of light. SERS increases the efficacy of Raman spectroscopy by utilizing plasmonic metal nanostructures to enhance signals by up to 108. Utilizing SERS detection for flowing solutions allows for minimal sample preparation, short analysis time, and sample recovery after analysis. This dissertation focuses on applying SERS in flow to low concentration samples to detect single molecules and analytes that are traditionally difficult to detect and differentiate. Chapter 1 introduces Raman and SERS as analytical tools and describes how these methods can be used for flow through analysis of both single molecules and sugars. Past literature of SERS in flow experiments and single molecule experiments are discussed to support the work shown in later chapters. Additional information regarding sugars, glycosylation, and chemometrics is provided. Chapter 2 focuses on a method for single molecule detection and quantification in flow. By utilizing fast acquisition SERS, a planar silver substrate, and chemometric analysis, the linear dynamic range of this technique is able to be lowered into the stochastic, or “event counting” regime instead of the traditional ensemble or “intensity based” regime. This allows for the limit of detection of Nile Blue A to be lowered by 16 times, and single molecules to be detected and counted. Chapter 3 discusses a method for detecting and differentiating monosaccharides in both flowing and static environments using a simple benchtop conjugation reaction, SERS detection, and chemometric methods for analysis. This method allows for detection of monosaccharides at micromolar concentrations and utilizes chemometric methods to differentiate between these isomeric molecules. Our results show that monosaccharides can be differentiated after conjugation with a boronic acid, allowing for simpler analysis of these difficult to detect and discriminate molecules. Chapter 4 focuses on applying the simple conjugation reaction and detection techniques from Chapter 3 to a more complex sample type, peptides modified with a single monosaccharide. Our results show that SERS can be used as a method to differentiate identical peptide chains that differ by only a single monosaccharide, but only if the monosaccharide in question has a sterically available cis-diol available for binding with a boronic acid. Chapter 5 provides a summary of this work and how the provided results may make an impact in the scientific community, especially in the areas of trace detection for toxicology, and glycan analysis for pharmacology and bioinformatics.
Zachary Schultz (Advisor)
Christopher Fang-Yen (Committee Member)
Robert Baker (Committee Member)
Abraham Badu-Tawiah (Committee Member)
122 p.
Analytical Chemistry; Chemistry
Raman spectroscopy; surface enhanced Raman spectroscopy; flow based analysis; sugar differentiation; single molecule detection; vibrational spectroscopy

Recommended Citations

Citations

  • Schorr, H. C. (2024). Characterization of rare events in flow using surface enhanced Raman spectroscopy (SERS) [Doctoral dissertation, Ohio State University]. OhioLINK Electronic Theses and Dissertations Center. http://rave.ohiolink.edu/etdc/view?acc_num=osu1721175705847462

    APA Style (7th edition)

  • Schorr, Hannah. Characterization of rare events in flow using surface enhanced Raman spectroscopy (SERS). 2024. Ohio State University, Doctoral dissertation. OhioLINK Electronic Theses and Dissertations Center, http://rave.ohiolink.edu/etdc/view?acc_num=osu1721175705847462.

    MLA Style (8th edition)

  • Schorr, Hannah. "Characterization of rare events in flow using surface enhanced Raman spectroscopy (SERS)." Doctoral dissertation, Ohio State University, 2024. http://rave.ohiolink.edu/etdc/view?acc_num=osu1721175705847462

    Chicago Manual of Style (17th edition)

osu1721175705847462
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This open access ETD is published by The Ohio State University and OhioLINK.
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