The effect of space charge in ion mobility spectrometry

Левин, М. Н.; Krisilov, A. V.; Zon, B. A.; Eiceman, Gary A.

doi:10.1007/s12127-014-0151-y

Cited by 10 publications

(6 citation statements)

References 23 publications

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“…Their hardware performance boundaries are constantly being pushed further, − especially in terms of resolving power. Fundamental parameters such as the influence of ion cloud densities and drift voltages on resolving power are as well being optimized in homemade drift tubes. − The improvements in resolving power of IM instruments lead to better separations of closely eluted compounds and to smaller drift time dispersions (i.e., a smaller IM peak width) with regards to the peak apex. While the IM measured quantities gain in precision and in accuracy, the calibration processes should avoid introducing uncertainties on CCS and K 0 values during the calibration procedure.…”

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confidence: 99%

Comprehensive Ion Mobility Calibration: Poly(ethylene oxide) Polymer Calibrants and General Strategies

et al. 2017

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Ion mobility (IM) is now a well-established and fast analytical technique. The IM hardware is constantly being improved, especially in terms of the resolving power. The Drift Tube (DTIMS), the Traveling Wave (TWIMS), and the Trapped Ion Mobility Spectrometry (TIMS) coupled to mass spectrometry are used to determine the Collision Cross-Sections (CCS) of ions. In analytical chemistry, the CCS is approached as a descriptor for ion identification and it is also used in physical chemistry for 3D structure elucidation with computational chemistry support. The CCS is a physical descriptor extracted from the reduced mobility (K) measurements obtainable only from the DTIMS. TWIMS and TIMS routinely require a calibration procedure to convert measured physical quantities (drift time for TWIMS and elution voltage for TIMS) into CCS values. This calibration is a critical step to allow interinstrument comparisons. The previous calibrating substances lead to large prediction bands and introduced rather large uncertainties during the CCS determination. In this paper, we introduce a new IM calibrant (CCS and K) using singly charged sodium adducts of poly(ethylene oxide) monomethyl ether (CHO-PEO-H) for positive ionization in both helium and nitrogen as drift gas. These singly charged calibrating ions make it possible to determine the CCS/K of ions having higher charge states. The fitted calibration plots exhibit larger coverage with less data scattering and significantly improved prediction bands and uncertainties. The reasons for the improved CCS/K accuracy, advantages, and limitations of the calibration procedures are also discussed. A generalized IM calibration strategy is suggested.

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confidence: 99%

Comprehensive Ion Mobility Calibration: Poly(ethylene oxide) Polymer Calibrants and General Strategies

et al. 2017

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“…This trend is consistent with the space charge broadening effect; as the terminal frequency of the sweep is decreased and therefore the resulting sweep rate is decreased, we observe band broadening in the ATD that is likely due to the increase in the ion population within the drift region. 47 For the remainder of experiments, a 5 min sweep with a terminal frequency of 5000 Hz resulting in a 16.65 Hz/s sweep was used unless otherwise noted.…”

Section: Optimization Of Multiplexing and Standard Gatingmentioning

confidence: 99%

Improving Ion Mobility Mass Spectrometry of Proteins through Tristate Gating and Optimization of Multiplexing Parameters

Butalewicz

Sanders

Clowers

et al. 2022

J. Am. Soc. Mass Spectrom.

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Coupling drift tube ion mobility (IM) to Fourier transform mass spectrometry (FT-MS) affords the opportunity for gas-phase separation of ions based on size and conformation with high-resolution mass analysis. However, combining IM and FT-MS is challenging because ions exit the drift tube on a much faster time scale than the rate of mass analysis. Fourier transform (FT) and Hadamard transform multiplexing methods have been implemented to overcome the duty-cycle mismatch, offering new avenues for obtaining high-resolution, high-mass-accuracy analysis of mobility-selected ions. The gating methods used to integrate the drift tube with the FT mass analyzer discriminate against the transmission of large, low-mobility ions owing to the well-known gate depletion effect. Tristate gating strategies have been shown to increase ion transmission for drift tube IM-FT-MS systems through implementation of dual ion gating, controlling the quantity and timing of ions through the drift tube to reduce losses of slow-moving ions. Here we present an optimized set of multiplexing parameters for tristate gating ion mobility of several proteins on an Orbitrap mass spectrometer and further report parameters for increased ion transmission and mobility resolution as well as decreased experimental times from 15 min down to 30 s. On average, peak intensities in the arrival time distributions (ATDs) for ubiquitin increased 2.1× on average, while those of myoglobin increased by 1.5× with a resolving power increase on average of 11%.

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“…Ionic species interact not only with the drift field (E d ), but also with each other's electric field. There are many excellent studies dealing with space charge effects in IMS, [53][54][55][56][57] including a recent paper by Eiceman and co-workers, 58 who developed and solved numerically a nonlinear integro-differential equation to account for the simultaneous dispersive effect of diffusion and Coulomb repulsion. They found that space charge effects become important when ion densities exceed 10 6 cm −3 , in accordance with previous findings.…”

Section: Intrinsic Contributors II Coulomb Repulsionmentioning

confidence: 99%