| The role of mass spectrometry in the chemical and biological sciences is ever evolving as there is an increasing interest to understand the biomolecular structure and interaction of proteins and their potential impact on human health. To this end, emerging techniques that complement or enhance mass spectrometric capabilities are of significant relevance.;While the impact of mass spectrometry in every field (e.g. proteomics, drug development, environmental, crop science, or petrochemical) has varied, increased accessibility of instrumentation and expertise to address relevant issues across disciplines will result in even greater acceptance of this powerful technology. Some compounds may not ionize by a predominant method, electrospray ionization (ESI) or matrix assisted laser desorption ionization (MALDI), but recently a number of ionization sources have been developed that further encompass more classes of molecules for mass spectrometric analysis. Limited sample availability is a practical issue which demands lower limits-of-detection. In efforts to address this, devices such as the ion funnel and the air amplifier are being developed to more efficiently transport ions within or into the mass spectrometer (respectively). With continued ionization source and instrumentation improvements, there will undoubtedly be additional physicians, scientists, and engineers who realize the great potential and benefit of using mass spectrometry to address questions related to their particular field of study.;This dissertation describes the utilization of Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS), which affords high resolving power and mass measurement accuracy, for the majority of ionization source developments. These ionization source efforts have been directed at improving current and emerging ionization techniques. A method for transporting neutral species for subsequent ionization termed remote analyte sampling, transport and ionization relay (RASTIR) has been developed and is described herein. Improvements for electrospray ionization have been realized using the air amplifier as it focuses and desolvates electrospray droplets; these mechanisms for improved ion abundance are investigated. An acoustic method for direct analysis of proteins and peptides from an oscillating surface is the premise of the radio frequency acoustic desorption ionization source. Collectively, this work aims to improve existing ionization techniques while investigating new avenues for biological mass spectrometry. |
