Department of Chemistry, Washington State University, Pullman, Washington 99164, United States.
J Am Soc Mass Spectrom. 2022 Oct 5;33(10):1858-1864. doi: 10.1021/jasms.2c00168. Epub 2022 Sep 6.
By casting the information regarding an ion population's mobility in the frequency domain, the coupling of time-dispersive ion mobility techniques is now imminently compatible with slower mass analyzers such as ion traps. Recent reports have detailed the continued progress toward maximizing the efficiency of the Fourier transform ion mobility-mass spectrometry (FT-IM-MS) experiments, but few reports have outlined the intersection between the practical considerations of implementation against the theoretical limits imposed by traditional signal processing techniques. One of the important concerns for Fourier-based multiplexing experiments is avoiding signal aliasing as a product of undersampled signals that may occur during data acquisition. In addition to traditional considerations such as detector sampling frequency, the limitations (i.e., maximum measurable drift time) imposed by experimental mass scan duration and the frequency sweep used for ion gate modulation must also be assessed. This work aims to connect the fundamental underpinnings of FT-IM-MS experiments and the associated experimental parameters that are encountered when coupling the comparatively fast separations in the mobility domain with the slower / scanning common for ion-trap mass analyzers. In addition to stating the relevant theory that applies to the FT-IM-MS experiment, this report highlights how aliased signals will manifest post Fourier transform in reconstructed arrival time distributions and calculated mobilities.
通过在频域中对离子群体迁移率的信息进行分析,现在时间分散型离子迁移率技术的耦合与离子阱等较慢的质量分析器完全兼容。最近的报告详细介绍了如何最大限度地提高傅里叶变换离子迁移率-质谱(FT-IM-MS)实验效率的持续进展,但很少有报告概述了实施的实际考虑因素与传统信号处理技术施加的理论限制之间的交点。基于傅里叶的多路复用实验的一个重要关注点是避免信号混叠,因为在数据采集过程中可能会出现欠采样信号的产物。除了传统的考虑因素,如探测器采样频率,实验质量扫描持续时间和离子门调制所用的频率扫描施加的限制(即最大可测量漂移时间)也必须进行评估。这项工作旨在连接 FT-IM-MS 实验的基本原理和相关的实验参数,当将迁移率域中相对较快的分离与离子阱质量分析器较慢/扫描速度耦合时,就会遇到这些参数。除了说明适用于 FT-IM-MS 实验的相关理论外,本报告还重点介绍了在重建到达时间分布和计算迁移率时,如何在傅里叶变换后显示混叠信号。