An IMS−IMS Analogue of MS−MS

Koeniger, Stormy L.; Merenbloom, Samuel I.; Valentine, Stephen J.; Jarrold, Martin F.; Udseth, Harold R.; Smith, Richard D.; Clemmer, David E.

doi:10.1021/ac051060w

Cited by 261 publications

(356 citation statements)

References 43 publications

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“…Thus, while the ion trapping efficiency is increased for He compared to N 2 , the physical space available for accumulation of higher charge states is reduced by space charge induced discrimination. The charge discrimination effects observed°in°the°experiment°as°highlighted°in°Figure°5°are consistent with the explanation described here and have also been observed in other IMS instruments that utilize ion°funnel°technology° [30];°further°optimization°of°the trap parameters will allow us to suppress the unwanted discrimination effects.…”

Section: Drift Gas Selection: He Versus Nsupporting

confidence: 82%

Ion mobility spectrometry—mass spectrometry performance using electrodynamic ion funnels and elevated drift gas pressures

Baker

Clowers

et al. 2007

J. Am. Soc. Mass Spectrom.

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The ability of ion mobility spectrometry coupled with mass spectrometry (IMS-MS) to characterize biological mixtures has been illustrated over the past eight years. However, the challenges posed by the extreme complexity of many biological samples have demonstrated the need for higher resolution IMS-MS measurements. We have developed a higher resolution ESI-IMS-TOF MS by utilizing high-pressure electrodynamic ion funnels at both ends of the IMS drift cell and operating the drift cell at an elevated pressure compared with that conventionally used. The ESI-IMS-TOF MS instrument consists of an ESI source, an hourglass ion funnel used for ion accumulation/injection into an 88 cm drift cell, followed by a 10 cm ion funnel and a commercial orthogonal time-of-flight mass spectrometer providing high mass measurement accuracy. It was found that the rear ion funnel could be effectively operated as an extension of the drift cell when the DC fields were matched, providing an effective drift region of 98 cm. The resolution of the instrument was evaluated at pressures ranging from 4 to 12 torr and ion mobility drift voltages of 16 V/cm (4 torr) to 43 V/cm (12 torr). An increase in resolution from 55 to 80 was observed from 4 to 12 torr nitrogen drift gas with no significant loss in sensitivity. The choice of drift gas was also shown to influence the degree of ion heating and relative trapping efficiency within the ion funnel. eveloping an effective analytical method to characterize extremely complex biological systems is one of the most difficult challenges in analytical chemistry. While many methods have been explored for this purpose, the high throughput capabilities of mass spectrometry (MS) and its ability to directly sample biomolecules out of solution using electrospray ionization (ESI) [1] are particularly suited to this task. Despite advances in this field, due to the broad range of analytes and their varying signal intensities within a complex sample, the ability to comprehensively detect a wide dynamic range of analytes in a single analysis remains limited. To address this problem, various separation methods capable of fractionation before MS analysis have been employed [2,3], specifically liquid chromatography (LC) [4] and ion mobility spectrometry (IMS) [5][6][7]. Thus, the methods of LC-MS [4], IMS-MS [8,9], and even LC-IMS-MS [10,11] have all been utilized in analyzing biological samples.While LC-MS allows analysis of the retention time and m/z for each biomolecule in a sample [12,13], a significant limitation to this technique is its speed since separations may take from minutes to several hours. On the other hand, IMS offers the basis for much faster separations when coupled with MS [8,9]. IMS is based on the fact that species with different collision cross sections travel with different velocities (i.e., ion mobilities) when they are pulled by a weak electric field through a drift cell filled with a buffer gas [14]. By coupling IMS to TOF MS, samples can be separated based on size and m/z very quickly due to ...

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Section: Drift Gas Selection: He Versus Nsupporting

confidence: 82%

Ion mobility spectrometry—mass spectrometry performance using electrodynamic ion funnels and elevated drift gas pressures

Baker

Clowers

et al. 2007

J. Am. Soc. Mass Spectrom.

Self Cite

127

149

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“…Moreover, the appearance of mixtures of fragment ions is likely not be limited to Leu-enkephalin, as others have observed multiple structures for particular CID product ions by ion mobility. 22,28 Finally, this study showed that the relative abundances of a 4 structures formed in CID are independent of the total energy deposited in the molecule, though this clearly does affect the individual fragment ion abundances in the CID mass spectrum. Moreover, extensive isomerization of a 4 structures takes place during activation, thereby apparently preventing structure-dependent CID.…”

Section: Discussionmentioning

confidence: 70%

On the Dynamics of Fragment Isomerization in Collision-Induced Dissociation of Peptides

et al. 2008

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The structures of peptide collision-induced dissociation (CID) product ions are investigated using ion mobility/ mass spectrometry techniques combined with theoretical methods. The cross-section results are consistent with a mixture of linear and cyclic structures for both b 4 and a 4 fragment ions. Direct evidence for cyclic structures is essential in rationalizing the appearance of fragments with scrambled (i.e., permutated) primary structures, as the cycle may not open up where it was initially formed. It is demonstrated here that cyclic and linear a 4 structures can interconvert freely as a result of collisional activation, implying that isomerization takes place prior to dissociation.

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“…These developments have also recently been adopted by Clemmer and coworkers. 16 Though ion transmission drastically improved as compared to earlier implementations of IMS-oTOF design, 17 we also note that lower efficiency of ion trapping/accumulation in the ion funnel still limits the ion utilization efficiency or duty cycle.…”

Section: Introductionmentioning

confidence: 83%

Multiplexed Ion Mobility Spectrometry-Orthogonal Time-of-Flight Mass Spectrometry

et al. 2007

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Ion mobility spectrometry (IMS) coupled to orthogonal time-of-flight mass spectrometry (oTOF) has shown significant promise for the characterization of complex biological mixtures. The enormous complexity of biological samples (e.g. from proteomics) and the need for both biological and technical analysis replicates imposes major challenges for multidimensional separation platforms in regard to both sensitivity and sample throughput. A major attraction of the IMS-TOF MS platform is separation speeds exceeding that of conventional condensed-phase separations by orders of magnitude. Known limitations of the IMS-TOF MS platforms include the need for extensive signal averaging due to factors that include significant ion losses in the IMS-TOF interface and an ion utilization efficiency of less than ~1% with continuous ion sources (e.g. ESI). We have developed a new multiplexed ESI-IMS-TOF mass spectrometer that enables lossless ion transmission through the IMS-TOF as well as a utilization efficiency of >50% for ions from the ESI source. Initial results with a mixture of peptides show a ~10-fold increase in signalto-noise ratio with the multiplexed approach compared to a signal averaging approach, with no reduction in either IMS or TOF MS resolution.

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An IMS−IMS Analogue of MS−MS

Cited by 261 publications

References 43 publications

Ion mobility spectrometry—mass spectrometry performance using electrodynamic ion funnels and elevated drift gas pressures

Ion mobility spectrometry—mass spectrometry performance using electrodynamic ion funnels and elevated drift gas pressures

On the Dynamics of Fragment Isomerization in Collision-Induced Dissociation of Peptides

Multiplexed Ion Mobility Spectrometry-Orthogonal Time-of-Flight Mass Spectrometry

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