Ion multiplexing: Maximizing throughput and signal to noise ratio for ion mobility spectrometry

Reinecke, Tobias; Naylor, Cameron N.; Clowers, Brian H.

doi:10.1016/j.trac.2019.03.014

Cited by 36 publications

(52 citation statements)

References 38 publications

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“…All ion multiplexing approaches generate data artifacts that arise during demultiplexing, due to the deviation of real data from what would be precisely predicted by the inverse transform (imperfect encoding) . The majority of artifacts observed in this work are of low abundance (<10% of the primary signal within each m / z extraction window) and located far enough away from the signal region of interest to not interfere with spectral interpretation, corresponding to their original (unprocessed) temporal locations based on the specific HT sequence used (see Figure B).…”

Section: Resultsmentioning

confidence: 95%

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Resolution of Isomeric Mixtures in Ion Mobility Using a Combined Demultiplexing and Peak Deconvolution Technique

Knochenmuss²,

et al. 2020

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A combined data acquisition and data processing strategy for improving the sensitivity and resolution of ion mobility measurements is described. This strategy is implemented on a commercially available drift tube ion mobility-mass spectrometry (IM-MS) instrument and utilizes both an existing ion multiplexing strategy to achieve up to an 8-fold gain in ion signal and a new postacquisition data reconstruction technique, termed “high resolution demultiplexing” (HRdm), to improve resolution in the ion mobility dimension. A series of isomeric mixtures were qualitatively investigated with HRdm, including biologically relevant lipids and carbohydrates, which were successfully resolved by HRdm, including two monosaccharide regioisomers which differed in drift time by only 0.8%. For a complex trisaccharide isomer mixture, HRdm was able to resolve 5 out of 6 components. An analysis of two-peak resolution (R pp) and peak-to-peak separation (ΔP) indicated that HRdm performs with an effective resolving power (R p) of between 180 to 250 for the highest deconvolution settings. Overall analysis times and drift time measurement precision were found to be unaffected between standard and HRdm processed data sets, which allowed statistically identical collision cross section values to be directly determined from all ion mobility spectra.

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Section: Resultsmentioning

confidence: 95%

“…Multiplexing strategies have been utilized to enhance the sensitivity and duty cycle of IMS instruments . Ion multiplexing is a strategy where multiple ion pulses are introduced to the IMS during each data acquisition cycle.…”

mentioning

confidence: 99%

Resolution of Isomeric Mixtures in Ion Mobility Using a Combined Demultiplexing and Peak Deconvolution Technique

Knochenmuss²,

et al. 2020

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“…As previously demonstrated, when constructing an ion modulation sequence using a PRBS generated through the traditional methods (e.g., prime and shift register techniques), the resultant sequence need not be applied exactly as generated . Rather, it is possible to scale the length of the sequence by an integer number to accommodate the time constraints of a given experiment. , For example if experimental parameters are not compatible with sequences that differ in length by a power of 2, it is possible to extend a sequence by simply inserting additional elements into the system. For example, a simple 4-bit sequence 000100110101111 extended, or oversampled by a factor of 3 would be 0 00 0 00 0 00 1 11 0 00 0 00 1 11 1 11 0 00 1 11 0 00 1 11 1 11 1 11 1 11 yielding a new sequence that is 45 elements long.…”

Section: Resultsmentioning

confidence: 99%

“…Evaluation of the new multiplexing technique was conducted by comparing the single injection experiment with three different multiplexing sequences corresponding to 6, 7, and 8-bit pseudo-random binary sequences (PRBS). An example sequence is provided in the Supporting Information, and a description of the sequence expansion approach [i.e., sequence oversampling (OS)] follows the concepts previously described. , …”

Section: Methodsmentioning

confidence: 99%

“…This range of analytes enabled performance evaluation with respect to sensitivity, dynamic range, and peak fidelity for multiply charged species. The underlying ion modulation strategy is governed by a pseudo random pulse sequence derived from a Hadamard matrix with unique autocorrelation properties. − The length of each Hadamard sequence scales with the power of 2 where a 5-bit sequence corresponds to a pseudo-random sequence with 31 element (2 n –1 , where n is the bit order of the sequence) . While effective Hadamard demultiplexing for reduced pressure ion mobility experiments has been realized for lower bit order sequences (4–6), the increased separation capacity of SLIM and extended arrival times require the use of higher bit orders (i.e., ≥7) along with a new class of deconvolution strategies.…”

Section: Introductionmentioning

confidence: 99%

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Masked Multiplexed Separations to Enhance Duty Cycle for Structures for Lossless Ion Manipulations

et al. 2021

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The experimental paradigm of one ion packet release per spectrum severely hinders throughput in broadband ion mobility spectrometry (IMS) systems (e.g., drift tube and traveling wave systems). Ion trapping marginally mitigates this problem, but the duty cycle deficit is amplified when moving to high resolution, long pathlength systems. As a consequence, new multiplexing strategies that maximize throughput while preserving peak fidelity are essential for high-resolution IMS separations [e.g., structures for lossless ion manipulations (SLIMs) and multi-pass technologies]. Currently, broadly applicable deconvolution strategies for Hadamard-based ion multiplexing are limited to a narrow range of modulation sequences and do not fully maximize the ion signal generated during separation across an extended path length. Compared to prior Hadamard deconvolution errors that rely upon peak picking or discrete error classification, the masked deconvolution matrix technique exploits the knowledge that Hadamard transform artifacts are reflected about the central, primary signal [i.e., the true arrival time distribution (ATD)]. By randomly inducing mathematical artifacts, it is possible to identify spectral artifacts simply by their high degree of variability relative to the core ATD. It is important to note that the deweighting approach using the masked deconvolution matrix does not make any assumptions about the underlying transform and is applicable to any multiplexing strategy employing binary sequences. In addition to demonstrating a 100-fold increase in the total number of ions detected, the effective deconvolution of data from 5, 6, 7, and 8-bit pseudo-random sequences expands the utility and efficiency of the SLIM platform.

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Recent developments in data acquisition, treatment and analysis with ion mobility‐mass spectrometry for lipidomics

et al. 2022

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Lipids are involved in many biological processes and their study is constantly increasing. To identify a lipid among thousand requires of reliable methods and techniques. Ion Mobility (IM) can be coupled with Mass Spectrometry (MS) to increase analytical selectivity in lipid analysis of lipids. IM-MS has experienced an enormous development in several aspects, including instrumentation, sensitivity, amount of information collected and lipid identification capabilities. This review summarizes the latest developments in IM-MS analyses for lipidomics and focuses on the current acquisition modes in IM-MS, the approaches for the pre-treatment of the acquired data and the subsequent data analysis. Methods and tools for the calculation of Collision Cross Section (CCS) values of analytes are also reviewed. CCS values are commonly studied to support the identification of lipids, providing a quasi-orthogonal property that increases the confidence level in the annotation of compounds and can be matched in CCS databases. The information contained in this review might be of help to new users of IM-MS to decide the adequate instrumentation and software to perform IM-MS experiments for lipid analyses, but also for other experienced researchers that can reconsider their routines and protocols.

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Ion multiplexing: Maximizing throughput and signal to noise ratio for ion mobility spectrometry

Cited by 36 publications

References 38 publications

Resolution of Isomeric Mixtures in Ion Mobility Using a Combined Demultiplexing and Peak Deconvolution Technique

Resolution of Isomeric Mixtures in Ion Mobility Using a Combined Demultiplexing and Peak Deconvolution Technique

Masked Multiplexed Separations to Enhance Duty Cycle for Structures for Lossless Ion Manipulations

Recent developments in data acquisition, treatment and analysis with ion mobility‐mass spectrometry for lipidomics

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