Photodissociation and Ion Trap Mass Spectrometry

在这项由化学系化学测量和成像计划资助的奖项中，布罗德贝特教授和她的学生将开发与化学衍生方法相结合的光解离方法，这种方法向分子中添加生色团和/或电荷位置，以修改离子碎裂模式。质谱学已经成为表征生物分子结构的最通用的方法之一，而提高质谱学策略的选择性仍然是当务之急。这项工作将遵循一个主题，旨在通过使用结合靶向选择性的离子激活方法来表征生物分子的结构，同时也建立一个框架来了解特定部位的发色团对离子激活的影响。主要目标包括评估电荷状态对解离效率的影响，结合发色团以提高解离效率，在分子中加入选择性可裂解的键，以及发展用于高通量蛋白质分析的光解离。除了这一提议的重要科学目标之外，未来科学家的教育也是具有长期影响的同样重要的成果。需要开发更好的分析工具，包括拟议工作中追求的质谱学策略，以阐明负责许多生物功能的分子结构，例如对抗病毒和心脏肌肉收缩的抗体。拟议工作的预期好处包括：1)在分析化学和生物质谱学领域对未来科学家进行培训和教育，以及2)开发基于激光的创新策略，以表征多肽、蛋白质、碳水化合物和核酸等生物分子的结构。

In this award, funded by the Chemical Measurement and Imaging Program of the Chemistry Division, Professor Brodbelt and her students will develop photodissociation in conjunction with chemical derivatization methods that add chromophores and/or charge sites to molecules in order to modify ion fragmentation patterns. Mass spectrometry has become one of the most versatile methods for structural characterization of biological molecules, and enhancing the selectivity of mass spectrometric strategies remains a priority. This work will follow a theme aimed at the structural characterization of biological molecules by using ion activation methods that incorporate targeted selectivity, while also building a framework for understanding the impact of site-specific chromophores on ion activation. The primary goals include the evaluation of charge state on dissociation efficiency, the attachment of chromophores to enhance dissociation efficiencies, the incorporation of selectively cleavable bonds into molecules, and the development of photodissociation for high throughput analysis of proteins. In addition to the important scientific goals of this proposal, the education of future scientists is an equally significant outcome with long-term impact. The development of better analytical tools, including the mass spectrometric strategies pursued in the proposed work, is needed to elucidate the structures of molecules responsible for many biological functions, such as antibodies that fight viruses and muscle contraction in the heart. The anticipated benefits arising from the proposed work include: 1) the training and education of future scientists in the area of analytical chemistry and biological mass spectrometry, and 2) the development of innovative laser-based strategies for structural characterization of biological molecules such as peptides, proteins, carbohydrates, and nucleic acids.