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High Lateral Resolution vs Molecular Preservation in near-IR fs-Laser Desorption Postionization Mass Spectrometry

机译:近红外fs激光解吸后电离质谱中的高横向分辨率与分子保留

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摘要

Ultrashort pulse length lasers operating in the near-infrared region show promise for submicrometer lateral resolution by laser desorption-based mass spectrometry (MS) imaging. However, these experiments must balance lateral resolution and molecular fragmentation since abundant atomic ions are observed at the high laser irradiances that can be generated by tightly focused ultrashort pulse laser beams. It is shown here that combining ultrashort pulse laser desorption with laser postionization (fs-LDPI) allows for a considerable increase of molecular ion signal while operating with lower laser irradiances, yielding the added benefit of reduced molecular fragmentation. This Letter presents several experimental results in support of the fs-LDPI approach for MS imaging. First, the lateral resolution for MS imaging of molecular species desorbed by similar to 75 fs, 800 nm laser pulses was determined to be <2 mu m for a simulated organic electronic device under vacuum. Next, the dependence of precursor ion survival on both desorption laser fluence and delay between desorption and photoionization laser pulses was observed for a small molecule desorbed from an organic multilayer that was originally devised as a model of a bacterial biofilm. When considered in light of recent results in the literature ( Milasinovic et al. J. Phys. Chem. C 2014 , DOI: 10.1021/jp504062u ), these experiments demonstrate the potential for submicrometer spatial resolution MS imaging by fs-LDPI.
机译:在近红外区域工作的超短脉冲长度激光器通过基于激光解吸的质谱(MS)成像显示出亚微米级横向分辨率的前景。但是,这些实验必须在横向分辨率和分子碎片之间取得平衡,因为在高激光辐照度下会观察到大量的原子离子,而高辐照度可以通过紧密聚焦的超短脉冲激光束产生。此处显示,将超短脉冲激光解吸与激光后离子化(fs-LDPI)结合使用,可在较低的激光辐照度下显着增加分子离子信号,从而带来减少分子碎片的额外好处。这封信提出了一些实验结果,以支持用于MS成像的fs-LDPI方法。首先,对于模拟有机电子设备在真空下,通过类似于75 fs,800 nm激光脉冲解吸的分子种类的MS成像的横向分辨率被确定为<2μm。接下来,对于从最初设计为细菌生物膜模型的有机多层中解吸出来的小分子,观察到了前驱物离子存活率对解吸激光通量以及解吸和光电离激光脉冲之间延迟的依赖性。当根据文献中的最新结果(Milasinovic等人,《化学物理杂志》 2014年,DOI:10.1021 / jp504062u)进行考虑时,这些实验证明了通过fs-LDPI进行亚微米空间分辨率MS成像的潜力。

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