CAREER: CDS&E: One- and Two-Dimensional Fourier Transform Approaches for Characterizing Nano-Assemblies with Ion Mobility-Mass Spectrometry

在化学系化学测量和成像计划的支持下，俄勒冈大学的James Prell教授正在开发使用质谱学准确确定大型聚合物和/或分子组件混合物的组成的分析方法。质谱学是一种化学分析工具，通常用于测量质量和确定许多类型的分子的结构。复杂混合物是工业和生化应用研究的主要目标，也是基础科学研究的主要目标。这些混合物的性质在很大程度上取决于它们不同成分的相对量以及它们的组装方式。从合成化学品到生物膜模型，使用质谱学或任何其他技术来表征这类系统可能具有极大的挑战性。普雷尔博士和他的团队正在开发新的方法来应对这些表征挑战，最终寻求促进对物理和化学特性的精确控制。该项目将最先进的质谱学与先进的数学和信号处理工具相结合。作为该项目的一部分而创建的公开可用的开源软件将提供给世界各地的研究人员用于分析这些类型的样本。同时，Prell博士试图通过一个以研究为基础的研讨会课程，增加来自不同背景的本科生对STEM研究的参与。这门课程的学生正在学习和实施向受众传达科学研究的策略，从中学到地区和国家STEM会议上的专业同事。Prell正在建立一个充满活力的综合研究和教育计划，以简化使用质谱学进行纳米级化学组件的分析，并增加来自代表性不足群体的STEM本科生的留校率和研究参与度。有三个具体的目标：1)建立基于傅里叶变换的方法来分析混合亚单位纳米组件，包括共聚物和脂蛋白组件的极端拥塞的电喷雾质谱学；2)引入基于傅立叶变换的二维测量工具，用于在先前的离子迁移率分离或普通傅立叶变换不足以处理的纳米组件的极端拥挤性的电喷雾质谱图中分离信号；以及3)增加本科生对科学研究的参与和交流。测量工具的目标是在与纳米组装研究相关的广泛应用中表征亚单位相互作用、组装形状和大小以及组装动力学。正在开发的软件是开放源代码和公开可用的，允许其他研究小组快速实施和调整。通过在俄勒冈大学为本科生实施1学分的研讨会课程，以这项研究得出的主题为原型，教育目标正在得到解决。这门课程的学生开发“电梯演讲”，以便交付给UO STEM桥梁项目；当地的初中和高中推广模块；以及提交给地区或国家科学会议的研究报告摘要。这些努力建立在PI在质谱学方面的专业知识和支持URM学生代表和纳入科学的经验的基础上，作为UO促进奇卡诺人/拉美裔和美洲原住民在科学中的分会的教师赞助商。该奖项反映了NSF的法定使命，并通过使用基金会的智力优势和更广泛的影响审查标准进行评估，被认为值得支持。

With support from the Chemical Measurement and Imaging Program in the Division of Chemistry, Professor James Prell at the University of Oregon is developing analytical methods for accurately determining the composition of mixtures of large polymers and/or molecular assemblies using mass spectrometry. Mass spectrometry is a tool for chemical analysis conventionally used to measure the mass and determine the structure of many types of molecules. Complex mixtures are a major target of research in industrial and biochemical applications as well as from the perspective of fundamental science. These mixtures can have properties that depend strongly on the relative amounts of their different constituents as well as how they are assembled. From synthetic chemicals to models of biological membranes, such systems can be extremely challenging to characterize using mass spectrometry or any other technique. Dr. Prell and his group are developing new approaches for these characterization challenges, ultimately seeking to facilitate precise control of physical and chemical properties. The project combines state-of-the-art mass spectrometry with advanced mathematical and signal processing tools. Publicly available, open-source software created as part of this project will be made available for researchers around the world to use in analyzing these types of samples. At the same time, Dr. Prell seeks to increase the participation of undergraduates from diverse backgrounds in STEM research through a research-based workshop course. Students in this course are learning and implementing strategies for communicating science research to audiences ranging from middle school through professional colleagues at regional and national STEM conferences.Dr. Prell is establishing a vigorous, integrated program of research and education to simplify the analysis of nanoscale chemical assemblies using mass spectrometry, and to increase the retention and research participation of STEM undergraduates from underrepresented groups. There are three specific aims: 1) to establish Fourier Transform-based methodology for analyzing extremely congested electrospray mass spectra of mixed-subunit nanoassemblies, including copolymers and lipoprotein assemblies; 2) to introduce two-dimensional Fourier Transform-based measurement tools for signal isolation in extremely congested electrospray mass spectra of nanoassemblies for which prior ion mobility separation or ordinary Fourier Transform are insufficient; and 3) to increase undergraduate participation in and communication of scientific research. Measurement tools target characterization of subunit interactions, assembly shape and size, and assembly kinetics in a wide variety of applications related to the study of nanoassemblies. Software being developed is open-source and publicly available, allowing rapid implementation and adaptation by other research groups. Educational goals are being addressed by implementing a 1-credit workshop course for undergraduates at the University of Oregon using themes drawn from this research as prototypes. Students in the course develop "elevator talks" for delivery to a UO STEM bridge program; local middle- and high school outreach modules; and a research presentation abstract for submission to a regional or national scientific conference. These efforts build off of the PI's expertise in mass spectrometry and experience supporting URM student representation and inclusion in science as a faculty sponsor of UO's chapter of the Society for the Advancement of Chicanos/Hispanics and Native Americans in Science.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.