Chemistry Department, Pennsylvania State University, University Park, PA, 16802, USA.
Smoluchowski Institute of Physics, Jagiellonian University, ulica Lojasiewicza 11, 30-348, Krakow, Poland.
J Am Soc Mass Spectrom. 2016 Sep;27(9):1476-82. doi: 10.1007/s13361-016-1423-z. Epub 2016 Jun 20.
The emergence of argon-based gas cluster ion beams for SIMS experiments opens new possibilities for molecular depth profiling and 3D chemical imaging. These beams generally leave less surface chemical damage and yield mass spectra with reduced fragmentation compared with smaller cluster projectiles. For nanoscale bioimaging applications, however, limited sensitivity due to low ionization probability and technical challenges of beam focusing remain problematic. The use of gas cluster ion beams based upon systems other than argon offer an opportunity to resolve these difficulties. Here we report on the prospects of employing CO2 as a simple alternative to argon. Ionization efficiency, chemical damage, sputter rate, and beam focus are investigated on model compounds using a series of CO2 and Ar cluster projectiles (cluster size 1000-5000) with the same mass. The results show that the two projectiles are very similar in each of these aspects. Computer simulations comparing the impact of Ar2000 and (CO2)2000 on an organic target also confirm that the CO2 molecules in the cluster projectile remain intact, acting as a single particle of m/z 44. The imaging resolution employing CO2 cluster projectiles is improved by more than a factor of two. The advantage of CO2 versus Ar is also related to the increased stability which, in addition, facilitates the operation of the gas cluster ion beams (GCIB) system at lower backing pressure. Graphical Abstract ᅟ.
基于氩气的气体团簇离子束在 SIMS 实验中的出现为分子深度剖析和 3D 化学成像开辟了新的可能性。与较小的团簇射弹相比,这些射弹通常会减少表面化学损伤,并产生碎片较少的质谱。然而,对于纳米级生物成像应用,由于低电离概率和束流聚焦的技术挑战,灵敏度有限仍然是一个问题。使用氩气以外的其他系统的气体团簇离子束提供了解决这些困难的机会。在这里,我们报告了使用 CO2 作为氩气的简单替代品的前景。我们使用一系列具有相同质量的 CO2 和 Ar 团簇射弹(团簇大小 1000-5000)在模型化合物上研究了电离效率、化学损伤、溅射率和束流聚焦。结果表明,这两种射弹在这些方面非常相似。比较 Ar2000 和(CO2)2000 对有机靶材影响的计算机模拟也证实,团簇射弹中的 CO2 分子保持完整,作为 m/z 44 的单个粒子起作用。使用 CO2 团簇射弹的成像分辨率提高了两倍以上。与 Ar 相比,CO2 的优势还与稳定性的提高有关,这也有助于在较低的背压下操作气体团簇离子束(GCIB)系统。