Analysis of Biological Molecules Using Stimulated Desorption Photoionization Mass Spectrometry
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Surface-assisted laser desorption/ionization mass spectrometry (SALDI MS) is a novel technique for direct analysis of organic and biological molecules. Amino acids, dipeptides, and organoselenium compounds were successfully detected by SALDI on carbon and silicon surfaces. Surface effects, solvent effects, temperature effects and pH effects were studied. A possible mechanism of SALDI is proposed based on observed results. In general, stimulated desorption results in neutral yields that are much larger than ion yields. Thus, we have exploited and further developed laser desorption single photon ionization mass spectrometry (LD/SPI MS) as a means of examining biomolecules. The experimental results clearly demonstrate that LD/SPI MS is a very useful and fast analysis method with uniform selectivity and high sensitivity. Selenium (Se) is an essential ultra-trace element in the human body. In efforts to obtain more useful information of selenium metabolites in human urine, mass determination of unknown organoselenium compounds in biological matrices using SALDI MS was investigated. In another approach, several selenium metabolites in human urine were successfully detected by LD/SPI MS. A HPLC-MS/MS method was also developed for a quantitative case study of selenium metabolites in human urine after ingestion of selenomethionine. Low-energy electrons (LEE, 3-20 eV) have been shown to induce single and double strand breaks (SSB and DSB) in plasmid DNA. To understand the genotoxic effects due to secondary species of high-energy radiation, we investigate the role of transient negative ions and the specificity in LEE-DNA damage by examining the neutral product yields using low electron stimulated dissociation SPI MS. The neutral yields as a function of incident electron energy are also correlated with the SSBs and DSBs measured using post-irradiation gel electrophoresis. The results provide further insight concerning the mechanisms of LEE-induced damage to DNA. Overall, this research provided an in-depth understanding of non-thermal surface processes and the development of new mass spectrometric techniques for the analysis of biomolecules.