Mass spectrometry, featured at high sensitivity, is an indispensable tool in the field of biophysics for studying intact protein and protein complex. Fourier Transform Ion Cyclotron Resonance (FTICR) mass spectrometer offers unparalleled resolving power and measured mass accuracy among various types of mass spectrometer. Further increase in mass resolving power can be achieved by increasing magnetic field strength and/or improving the performance of the mass analyzer (i.e., FTICR ion trap). Increasing the magnetic field strength is nontrivial in terms of fabrication techniques and economic aspect. This work is to increase the resolving power by the latter approach: developing a new FTICR ion trap of superior performance to increase the resolving power without increasing the magnetic field strength. The new FTICR ion trap development has been conducted in three aspects corresponding to the mass analyzer's three basic functions: trapping, excitation and detection. Chapter Two describes comprehensive comparisons of two latest FTICR ion traps for which the trapping electric fields are generated based on two different principles: statically harmonized electric potential and dynamically harmonized electric potential. The evaluation of the two FTICR ion traps is carried out by simulation and experiments. The simulation is based on finite difference method (FDM). The experiments are conducted on a custom-built 9.4 Tesla FTICR instrument. All of the advantages of the two ion traps have been incorporated into the new FTICR ion trap design. Chapter Three describes a novel electrical circuit which enables conducting excitation and detection functions on the same electrodes of FTICR ion trap. This circuit eliminates the restriction on excitation and detection electrode angular extents, which permits more efficient choice of electrode geometries for excitation and detection simultaneously. The circuit laid the foundation for the new FTICR ion trap design. Chapter Four demonstrates the new FTICR ion trap which possesses optimal excitation electric fields and ability of conducting the second frequency-multiple detection, founded on the optimized geometry and the associated circuit. The optimized geometry improves the radial and axial uniformity of excitation electric field which promotes large post-excitation radii desired by frequency-multiples detection. The circuit for conducting excitation and detection on same electrodes establishes the feasibility for such intended geometry modifications. The design of the new FTICR ion trap is initiated by theoretical analysis, guided by simulation and evaluated by experiments. The new FTICR ion trap not only meet the design target (i.e., doubling the resolving power under the same magnetic field strength), but also provide an approach of conducting even higher frequency-multiples detection for FTICR MS in future. Chapter Five describes an application of ultra-high resolving power mass spectrometry in the field of biophysics: the ultra-high resolution Hydrogen Deuterium Exchange Mass Spectrometry (HDX-MS) experiments. Compared to the conventional HDX-MS experiments, ultra-high resolution MS can eliminate the potential errors in deuterium uptake calculation and largely accelerate the data processing. Chapter Six introduces one of the future research projects: the third frequency-multiple detection for FTICR MS. It is a follow-up of this doctoral work and is being investigated in our group. The corresponding circuit diagram is presented. / A Dissertation submitted to the Institute of Molecular Biophysics in partial fulfillment of the Doctor of Philosophy. / Spring Semester, 2015. / January 28, 2015. / Includes bibliographical references. / Alan G. Marshall, Professor Directing Dissertation; Linda S. DeBrunner, University Representative; Timothy M. Logan, Committee Member; William S. Oates, Committee Member; Scott Stagg, Committee Member.
| Identifer | oai:union.ndltd.org:fsu.edu/oai:fsu.digital.flvc.org:fsu_253443 |
| Contributors | Chen, Tong (authoraut), Marshall, Alan G., 1944- (professor directing dissertation), DeBrunner, Linda S. (Linda Sumners) (university representative), Logan, Timothy M., 1961- (committee member), Oates, William S. (committee member), Stagg, Scott (committee member), Florida State University (degree granting institution), College of Arts and Sciences (degree granting college), Program in Molecular Biophysics (degree granting department) |
| Publisher | Florida State University, Florida State University |
| Source Sets | Florida State University |
| Language | English, English |
| Detected Language | English |
| Type | Text, text |
| Format | 1 online resource (74 pages), computer, application/pdf |
| Rights | This Item is protected by copyright and/or related rights. You are free to use this Item in any way that is permitted by the copyright and related rights legislation that applies to your use. For other uses you need to obtain permission from the rights-holder(s). The copyright in theses and dissertations completed at Florida State University is held by the students who author them. |
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