Pseudorandom sequence modifications for ion mobility orthogonal time-of-flight mass spectrometry
Pseudorandom sequence modifications for ion mobility orthogonal time-of-flight mass spectrometry
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DOI：
10.1021/ac7022712
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发表时间：
2008-04-01
影响因子：
7.4
通讯作者：
Smith, Richard D.
中科院分区：
文献类型：
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作者：
Clowers, Brian H.;Belov, Mikhail E.;Smith, Richard D.
由于从连续离子源采样的离子迁移谱 (IMS) 实验固有的低占空比，因此已经开发了一系列实验进展以最大限度地提高离子利用效率。在离子迁移漂移管之前使用离子捕获和累积方法已证明比连续源的离散采样有显着的增益，但传统上依赖信号平均 (SA) 来获得分析上有用的信噪比 (SNR)。基于 Hadamard 变换的多重 (MP) 技术提供了另一种实验方法，通过该方法可以将离子利用率从大约 1% 提高到大约 50%。最近，我们的研究小组展示了一种独特的多重离子淌度飞行时间 (MP-IMS-TOF) 方法，该方法结合了离子捕获功能，可以将离子利用率提高到 50% 以上。然而，使用这种实验方法对多路复用信号进行频谱重建需要使用特定于样本的加权设计。这种通用加权设计已被证明可以使用这种 MP 技术显着提高离子利用效率，但不能普遍应用。通过修改用于 MP 实验的离子捕获和伪随机序列 (PRS)，我们消除了对复杂加权矩阵的需要。对于简单和复杂的混合物，与 SA-IMS-TOF 方法相比，通常观察到 SNR 增强高达 13。此外，与传统的 HT-IMS 实验相比，这种新型 PRS 使每单位时间的离子门脉冲数量增加了 2 倍。
Due to the inherently low duty cycle of ion mobility spectrometry (IMS) experiments that sample from continuous ion sources, a range of experimental advances have been developed to maximize ion utilization efficiency. The use of ion trapping and accumulation approaches prior to the ion mobility drift tube has demonstrated significant gains over discrete sampling from continuous sources but have traditionally relied upon a signal averaging (SA) to attain analytically useful signal-to-noise ratios (SNR). Multiplexed (MP) techniques based upon the Hadamard transform offer an alternative experimental approach by which ion utilization efficiency can be elevated from similar to 1 to similar to 50%. Recently, our research group demonstrated a unique multiplexed ion mobility time-of-flight (MP-IMS-TOF) approach that incorporates ion trapping and can extend ion utilization efficiency beyond 50%. However, the spectral reconstruction of the multiplexed signal using this experiment approach requires the use of sample-specific weighting designs. Such general weighting designs have been shown to significantly enhance ion utilization efficiency using this MP technique, but cannot be universally applied. By modifying both the ion trapping and the pseudorandom sequence (PRS) used for the MP experiment, we have eliminated the need for complex weighting matrices. For both simple and complex mixtures, SNR enhancements of up to 13 were routinely observed as compared to the SA-IMS-TOF approach. In addition, this new class of PRS provides a 2-fold enhancement in the number of ion gate pulses per unit time compared to the traditional HT-IMS experiment.