Russell Zachary E, Chen Evan X, Amsden Jason J, Wolter Scott D, Danell Ryan M, Parker Charles B, Stoner Brian R, Gehm Michael E, Brady David J, Glass Jeffrey T
Department of Electrical and Computer Engineering, Duke University, Durham, NC, 27708, USA.
J Am Soc Mass Spectrom. 2015 Feb;26(2):248-56. doi: 10.1007/s13361-014-1051-4. Epub 2014 Dec 16.
In mass spectrometer design, there has been a historic belief that there exists a fundamental trade-off between instrument size, throughput, and resolution. When miniaturizing a traditional system, performance loss in either resolution or throughput would be expected. However, in optical spectroscopy, both one-dimensional (1D) and two-dimensional (2D) aperture coding have been used for many years to break a similar trade-off. To provide a viable path to miniaturization for harsh environment field applications, we are investigating similar concepts in sector mass spectrometry. Recently, we demonstrated the viability of 1D aperture coding and here we provide a first investigation of 2D coding. In coded optical spectroscopy, 2D coding is preferred because of increased measurement diversity for improved conditioning and robustness of the result. To investigate its viability in mass spectrometry, analytes of argon, acetone, and ethanol were detected using a custom 90-degree magnetic sector mass spectrometer incorporating 2D coded apertures. We developed a mathematical forward model and reconstruction algorithm to successfully reconstruct the mass spectra from the 2D spatially coded ion positions. This 2D coding enabled a 3.5× throughput increase with minimal decrease in resolution. Several challenges were overcome in the mass spectrometer design to enable this coding, including the need for large uniform ion flux, a wide gap magnetic sector that maintains field uniformity, and a high resolution 2D detection system for ion imaging. Furthermore, micro-fabricated 2D coded apertures incorporating support structures were developed to provide a viable design that allowed ion transmission through the open elements of the code.
在质谱仪设计中,一直存在一种历史观念,即仪器尺寸、通量和分辨率之间存在根本的权衡。当对传统系统进行小型化时,预计分辨率或通量会有性能损失。然而,在光学光谱学中,一维(1D)和二维(2D)孔径编码已被使用多年来打破类似的权衡。为了为恶劣环境现场应用提供可行的小型化途径,我们正在扇形质谱分析中研究类似的概念。最近,我们证明了一维孔径编码的可行性,在此我们首次对二维编码进行研究。在编码光学光谱学中,二维编码更受青睐,因为增加了测量多样性,可改善结果的条件并提高稳健性。为了研究其在质谱分析中的可行性,使用了一台定制的90度扇形磁质谱仪,该质谱仪结合了二维编码孔径,对氩气、丙酮和乙醇的分析物进行了检测。我们开发了一个数学正向模型和重建算法,以成功地从二维空间编码的离子位置重建质谱。这种二维编码在分辨率降低最小的情况下使通量提高了3.5倍。在质谱仪设计中克服了几个挑战以实现这种编码,包括需要大的均匀离子通量、一个保持场均匀性的宽间隙扇形磁场以及一个用于离子成像的高分辨率二维检测系统。此外,还开发了包含支撑结构的微加工二维编码孔径,以提供一种可行的设计,使离子能够通过编码的开放元件传输。