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复用条件对哈达玛变换离子迁移谱中伪信号及解码数据信噪比的影响

Influence of multiplexing conditions on artefact signal and the signal-to-noise ratio in the decoded data in Hadamard transform ion mobility spectrometry.

作者信息

Sarycheva Anastasia, Adamov Alexey, Poteshin Sergey S, Lagunov Sergey S, Sysoev Alexey A

机构信息

Molecular Physics Department, National Research Nuclear University MEPhI (Moscow Engineering Physics Institute), Moscow, Russia.

Linantec, Ltd, Moscow, Russia.

出版信息

Eur J Mass Spectrom (Chichester). 2020 Jun;26(3):204-212. doi: 10.1177/1469066719900763. Epub 2020 Jan 24.

Abstract

In Hadamard transform ion mobility spectrometry (HT IMS), the signal-to-noise ratio is always lower for non-modified pseudorandom sequences than for modified sequences. Since the use of non-modified modulating pseudorandom sequences is strategically preferable from a duty cycle standpoint, we investigated the change in the interference signal when transitioning from non-modified modulating sequences to sequences modified by the addition of 1,3,5 and 7 zeros. The interfering signal in HT IMS with modified pseudorandom sequences was shown to be mainly random noise for all the cases except for modifying by incorporation of 1 zero. For standard samples of tetraalkylammonium halides, modulation by non-modified pseudorandom sequences is beneficial in the case of small numbers of averaged spectra (below ∼40 averaged spectra compared to any modified pseudorandom sequences except for 1 zero modified and below ∼200 averaged spectra compared to signal averaging ion mobility spectrometry) and worsens the signal-to-noise ratio in the case of large numbers of averaged spectra. Contrarily, modulation by modified pseudorandom sequences is beneficial for any number of averaged spectra, except for very small ones (below 15 averaged spectra compared to modulation by non-modified sequences). Pseudorandom sequence modified with 1 zero incorporation is beneficial in the case of below ∼400 averaged spectra compared to any modified and non-modified pseudorandom sequences. The signal-to-noise ratio in conventional signal averaging mode ion mobility spectrometry is affected by random noise, whereas the HT IMS with non-modified pseudorandom sequences was demonstrated to be primarily affected by a systematic noise-like artefact signal. Because noise-like artefact signals were found to be reproducible, predicting models for interference signals could be generated to improve signal-to-noise ratio. This is significant because non-modified modulating sequences are limited by their poor signal-to-noise ratio. This improvement would increase the viability of non-modified modulating sequences which are preferred because of their higher sample utilization efficiency.

摘要

在哈达玛变换离子迁移谱(HT IMS)中,未修饰的伪随机序列的信噪比总是低于修饰序列。由于从占空比的角度来看,使用未修饰的调制伪随机序列在策略上更可取,因此我们研究了从不修饰的调制序列过渡到添加1、3、5和7个零进行修饰的序列时干扰信号的变化。结果表明,除了掺入1个零进行修饰的情况外,在所有情况下,具有修饰伪随机序列的HT IMS中的干扰信号主要是随机噪声。对于卤化四烷基铵的标准样品,在平均光谱数量较少时(与除1个零修饰之外的任何修饰伪随机序列相比,低于约40个平均光谱;与信号平均离子迁移谱相比,低于约200个平均光谱),使用未修饰的伪随机序列进行调制是有益的,而在平均光谱数量较多时,会使信噪比变差。相反,对于任何数量的平均光谱,除了非常少的情况(与未修饰序列的调制相比,低于15个平均光谱)外,使用修饰伪随机序列进行调制都是有益的。与任何修饰和未修饰的伪随机序列相比,掺入1个零修饰的伪随机序列在平均光谱数量低于约400个时是有益的。传统信号平均模式离子迁移谱中的信噪比受随机噪声影响,而具有未修饰伪随机序列的HT IMS被证明主要受类似系统噪声的伪像信号影响。由于发现类似噪声的伪像信号是可重现的,因此可以生成干扰信号的预测模型以提高信噪比。这一点很重要,因为未修饰的调制序列受其较差的信噪比限制。这种改进将提高未修饰调制序列的可行性,由于其更高的样品利用效率,未修饰调制序列是更可取的。

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