Abstract:The utility of ion mobility spectrometry (IMS) for separation of mixtures and structural characterization of ions has been demonstrated extensively, including in biological and nanoscience contexts. A major attraction of IMS is its speed, several orders of magnitude greater than that of condensed-phase separations. Nonetheless, IMS combined with mass spectrometry (MS) has remained a niche technique, substantially because of limited sensitivity resulting from ion losses at the IMS-MS junction. We have developed… Show more
“…29,33 If the width of the ion packets exceeds the inner diameter of the drift tube prior to its arrival at the IMS terminus, then ions are lost and ion transmission efficiency is reduced. The transmission efficiency through the IMS space alone was assumed to be 100% when Tang et al demonstrated near-perfect ion transfer through an ion funnel interface for ESI-IMS-MS. 34 Sysoev el al also concluded ion loss during transmission through IMS tube was minimal when they obtained similar signals with and without a modular IMS inserted between ESI-MS. 35 Gillig et al simulated ion trajectories inside the drift tube and showed that ions were transferred without any loss through the drift tube when they reported an ion focusing guide for MALDI-IMS-MS. 36 However to our knowledge, no direct empirical data has been reported to demonstrate ion transmission is close to 100% in IMS tube.…”
Reduced flow-rate electrospray ionization has been proven to provide improved sensitivity, less background noise, and improved limits of detections for ESI-MS analysis. Miniaturizing the ESI source from conventional electrospray to micro-electrospray and further down to nanoelectrospray has resulted in higher and higher sensitivity. However, when effects of flow rate were investigated for atmospheric pressure ESI-IMS using a nanospray emitter, a striking opposite result was observed. The general tendency we observed in ESI-IMS was that higher flow rate offered higher ion signal intensity throughout a variety of conditions investigated. Thus further efforts were undertaken to rationalize these contradictory results. It is well accepted that decreased flow rate increases both ionization efficiency and transmission efficiency thus improves ion signal in ESI-MS. However, our study revealed that decreased flow rate results in decreased ion signal because ion transfer is constant no matter how flow rate changes in ESI-IMS. Since ion transfer is constant in atmospheric pressure ESI-IMS, ionization efficiency can be studied independently, which otherwise is not possible in ESI-MS where both ionization efficiency and transmission efficiency vary as conditions alter. In this report, we present a systematic study on signal intensity and ionization efficiency at various experimental conditions using ESI-IMS and demonstrated the ionization efficiency as a function of flow rate, analyte concentration, and solvent composition.
“…29,33 If the width of the ion packets exceeds the inner diameter of the drift tube prior to its arrival at the IMS terminus, then ions are lost and ion transmission efficiency is reduced. The transmission efficiency through the IMS space alone was assumed to be 100% when Tang et al demonstrated near-perfect ion transfer through an ion funnel interface for ESI-IMS-MS. 34 Sysoev el al also concluded ion loss during transmission through IMS tube was minimal when they obtained similar signals with and without a modular IMS inserted between ESI-MS. 35 Gillig et al simulated ion trajectories inside the drift tube and showed that ions were transferred without any loss through the drift tube when they reported an ion focusing guide for MALDI-IMS-MS. 36 However to our knowledge, no direct empirical data has been reported to demonstrate ion transmission is close to 100% in IMS tube.…”
Reduced flow-rate electrospray ionization has been proven to provide improved sensitivity, less background noise, and improved limits of detections for ESI-MS analysis. Miniaturizing the ESI source from conventional electrospray to micro-electrospray and further down to nanoelectrospray has resulted in higher and higher sensitivity. However, when effects of flow rate were investigated for atmospheric pressure ESI-IMS using a nanospray emitter, a striking opposite result was observed. The general tendency we observed in ESI-IMS was that higher flow rate offered higher ion signal intensity throughout a variety of conditions investigated. Thus further efforts were undertaken to rationalize these contradictory results. It is well accepted that decreased flow rate increases both ionization efficiency and transmission efficiency thus improves ion signal in ESI-MS. However, our study revealed that decreased flow rate results in decreased ion signal because ion transfer is constant no matter how flow rate changes in ESI-IMS. Since ion transfer is constant in atmospheric pressure ESI-IMS, ionization efficiency can be studied independently, which otherwise is not possible in ESI-MS where both ionization efficiency and transmission efficiency vary as conditions alter. In this report, we present a systematic study on signal intensity and ionization efficiency at various experimental conditions using ESI-IMS and demonstrated the ionization efficiency as a function of flow rate, analyte concentration, and solvent composition.
“…26 The timing sequence of the ion mobility experiment was synchronized with the pulsing frequency of the Q-TOF and controlled using a PCI-6711 timing card (National Instruments, Austin, TX).…”
Section: Ion Mobility-quadrupole-time Of Flight Mass Spectrometermentioning
confidence: 99%
“…Improvements to ion transmission through an mobility drift tube were achieved for the continuous mode (i.e., no IMS separation) by combining electrodynamic ion funnels with the IMS drift tube. 26 More recently, our laboratory demonstrated the use of a novel IFT design operated at 1 Torr in combination with a time-of-flight (TOF) mass spectrometer equipped with analog-to-digital converter (ADC) detection. 29 The results showed that improvements in ion packet charge density were accompanied by 10-to 30-fold gains in SNR with respect to signals obtained using the same instrument operating in the continuous mode.…”
Conventional ion mobility spectrometers that sample ion packets from continuous sources have traditionally been constrained by an inherently low duty cycle. As such, ion utilization efficiencies have been limited to <1% in order to maintain instrumental resolving power. Using a modified electrodynamic ion funnel, we demonstrated the ability to accumulate, store, and eject ions in conjunction with ion mobility spectrometry (IMS), which elevated the charge density of the ion packets ejected from the ion funnel trap (IFT) and provided a considerable increase in the overall ion utilization efficiency of the IMS instrument. A 7-fold increase in signal intensity was revealed by comparing continuous ion beam current with the amplitude of the pulsed ion current in IFT-IMS experiments using a Faraday plate. Additionally, we describe the IFT operating characteristics using a time-of-flight mass spectrometer attached to the IMS drift tube.
“…Tang et al have recently reported on ion lossless IMS-MS separations with an IMS drift tube incorporated between two electrodynamic ion funnels. 14 In that experiment, ions were trapped in an "hourglass" ion funnel for 50 to 100 ms at an elevated pressure of 4 torr and then gated into the IMS drift tube in short 50 μs pulses. At the exit of the IMS drift tube, ion packets, spatially dispersed mainly due to thermal diffusion 15 , were captured by a regular ion funnel followed by a short collisional quadrupole.…”
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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