3D Momentum Imaging of Matrix-Assisted Laser Desorption/Ionization (MALDI) in the Time Domain

时域基质辅助激光解吸/电离 (MALDI) 的 3D 动量成像

• 批准号: 2107860
• 负责人: Wen Li
• 金额: $ 45万
• 依托单位: Wayne State University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2021
• 资助国家: 美国
• 起止时间: 2021-09-01 至 2024-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2107860&HistoricalAwards=false
• 关键词: 3D; Momentum; Imaging; Matrix; Assisted

With support from the Chemical Measurement and Imaging Program in the Division of Chemistry, Professor Wen Li and his group at Wayne State University are undertaking fundamental studies related to mass spectrometry, a powerful method of chemical analysis with broad applications in biology, chemistry, and medicine. Specifically, the Li group is studying the mechanism of Matrix-Assisted Laser Desorption/Ionization (MALDI), a widely employed technique for producing ions that are subjected to mass analysis. Despite decades of research effort, knowledge of the details of the underlying mechanism of MALDI remains imperfect. This project aims to enhance our understanding of these details using newly developed research tools to provide unprecedented insights into the MALDI process. It is expected that improved insight may lead to improved sensitivity. Students engaged in these studies will gain excellent interdisciplinary training. Dr. Li is also active in outreach to high school students, in efforts to enhance their interest in career paths in science.The project aims to enhance understanding of the mechanisms of primary ionization in MALDI and aims to improve the sensitivity of the technique in detecting complex and large molecules of biological relevance. Femto- and picosecond lasers coupled with high-resolution three-dimensional momentum imaging of both ejected electrons and ions will be employed with the goal of providing unprecedented details about ionization dynamics. Schemes using ultrashort pulse pumping to reduce the sample loss to neutral desorption will be devised with an aim of significantly increasing sensitivity. Specifically, three projects will be integrated to unravel the complex dynamics: 1) developing a novel ultrafast thermometry method based on electron imaging with a resolution of tens of picoseconds for measuring the time-resolved temperatures of samples; 2) carrying out time-resolved thermometry measurements on DHB to assess the validity of various models; and 3) investigating a new laser desorption/ionization mechanism driven by femtosecond pulses. These studies are expected to illuminate details of the initial ionization process and may lead to enhancement of MALDI sensitivity.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.

韦恩州立大学的李文教授和他的小组在化学系化学测量和成像项目的支持下，正在进行与质谱法有关的基础研究。质谱法是一种强大的化学分析方法，在生物学、化学和医学方面有广泛的应用。具体来说，Li小组正在研究基质辅助激光解吸/电离（MALDI）的机制，这是一种广泛使用的用于产生进行质量分析的离子的技术。尽管数十年的研究努力，MALDI的潜在机制的细节知识仍然不完善。该项目旨在通过使用新开发的研究工具来增强我们对这些细节的理解，从而为MALDI过程提供前所未有的见解。预期改善的洞察力可导致改善的灵敏度。 从事这些研究的学生将获得优秀的跨学科培训。 李博士还积极与高中生开展外联活动，努力提高他们对科学职业道路的兴趣。该项目旨在提高对MALDI中初级电离机制的理解，并旨在提高该技术在检测生物相关的复杂和大分子方面的灵敏度。将采用飞秒和皮秒激光器，再加上高分辨率的三维动量成像的喷射电子和离子，其目标是提供有关电离动力学的前所未有的细节。计划使用超短脉冲泵浦，以减少样品损失中性解吸将设计与显着提高灵敏度的目的。具体而言，将整合三个项目来揭示复杂的动力学：1）开发一种基于电子成像的新型超快测温方法，其分辨率为数十皮秒，用于测量样品的时间分辨温度; 2）对DHB进行时间分辨测温测量，以评估各种模型的有效性;研究了飞秒脉冲驱动的激光解吸电离新机制。这些研究有望阐明初始电离过程的细节，并可能导致MALDI灵敏度的提高。该奖项反映了NSF的法定使命，并已被认为值得通过使用基金会的智力价值和更广泛的影响审查标准进行评估的支持。

项目成果

Three-dimensional (3D) moment imaging with a USB3 oscilloscope.

使用 USB3 示波器进行三维 (3D) 矩成像。

• DOI: 10.1063/5.0155903
• 发表时间: 2023
• 期刊: The Review of scientific instruments
• 作者: Yasashri Ranathunga;T. Olowolafe;S. Lee;Wen Li
• 通讯作者: Wen Li

Picosecond vs Femtosecond: Are All Laser Desorption Ionizations Created Equal?

皮秒与飞秒：所有激光解吸电离作用都相同吗？

• DOI: 10.1021/acs.jpcc.2c06573
• 发表时间: 2022
• 期刊: The Journal of Physical Chemistry C
• 作者: Stewart, Gabriel A.;Debrah, Duke;Ranathunga, Yasashri;Olowolafe, Temitayo A.;Schlegel, H. Bernhard;Lee, Suk Kyoung;Li, Wen
• 通讯作者: Li, Wen