High kinetic energy ion mobility spectrometry (HiKE-IMS) allows for sensitive trace gas analysis within seconds, mitigating many disadvantages of standard ion mobility spectrometers through operation at reduced pressure and high electric field strengths. However, these advantages usually come at the cost of reduced resolving power, ranging from a maximum of 75 down to 50 at a reduced field strength of 120 Td for the original device. In this work, we present an extended theory for HiKE-IMS resolving power and a novel tristate ion shutter principle able to achieve initial ion packet widths of 1 μs without significant mobility discrimination. Such an ultrashort injection time allows for improving the resolving power of the HiKE-IMS to 140 for a wide range of reduced electric field strengths. With this resolving power, separating all ion species generated from a mixture of benzene, toluene, and xylene is possible. Furthermore, a resolving power of 140 is sufficient to partially separate isotopologues under high electric field strengths.
Abstract. Split-ring resonators are electrical circuits, which enable highly sensitive readout of split capacity changes via a measurement of the shift in the resonance frequency. Thus, functionalization of the split allows the development of biosensors, where selective molecular binding causes a change in permittivity and therefore a change in split capacity. In this work, we present a novel approach using transmission line theory to describe the dependency between permittivity of the sample and resonance frequency. This theory allows the identification of all relevant parameters of a split-ring resonator and thus a target-oriented optimization process. Hereby all setup optimizations are verified with measurements. Subsequently, the split of a resonator is functionalized with aptamers and the sensor response is investigated. This preliminary experiment shows that introducing the target protein results in a shift in the resonance frequency caused by a permittivity change due to aptamer-mediated protein binding, which allows selective detection of the target protein.
Corona discharge ionization sources are often used in ion mobility spectrometers (IMS) when a non-radioactive ion source with high ion currents is required. Typically, the corona discharge is followed by a reaction region where analyte ions are formed from the reactant ions. In this work, we present a simple yet sufficiently accurate model for predicting the ion current available at the end of this reaction region when operating at reduced pressure as in High Kinetic Energy Ion Mobility Spectrometers (HiKE-IMS) or most IMS-MS instruments. It yields excellent qualitative agreement with measurement results and is even able to calculate the ion current within an error of 15%. Additional interesting findings of this model are the ion current at the end of the reaction region being independent from the ion current generated by the corona discharge and the ion current in High Kinetic Energy Ion Mobility Spectrometers (HiKE-IMS) growing quadratically when scaling down the length of the reaction region. Graphical Abstract ᅟ.
Due to their high sensitivity and compact design, ion mobility spectrometers are widely used to detect toxic industrial chemicals (TICs) in air. However, when analyzing complex gas mixtures, classical ion mobility spectrometry (IMS) suffers from false-positive rates due to limited resolving power or false-negative rates caused by competitive ion−molecule reactions and the resulting suppression of certain analyte ions. To overcome these limitations, high-kinetic energy IMS (HiKE-IMS) was introduced some years ago. In contrast to classical IMS, HiKE-IMS is operated at decreased pressures of 20•••60 mbar and high reduced electric field strengths E/N of up to 120 Td. Under these conditions, the influence of competitive ion−molecule reactions on the prevailing ion population should be less pronounced, thus reducing false negatives. Additionally, effects such as fragmentation and field-dependent ion mobility may help to reduce false positives. In this work, the capabilities and limitations of HiKE-IMS in the field of on-site detection of the volatile TICs NH 3 , HCN, H 2 S, HCl, NO 2 , Cl 2 , and SO 2 are evaluated for the first time. Based on the limits of detection and the extent of spectral and chemical cross-sensitivities in gas mixtures, the results obtained for HiKE-IMS are compared with those obtained for classical IMS. It is shown that HiKE-IMS is less sensitive in comparison to classical IMS. However, when used for TIC detection, the reduced sensitivity of HiKE-IMS is not a major drawback. With values around 1 ppm v , the achievable limits of detection for almost all TICs are below the AEGL-2 (4h) levels. Furthermore, in comparison to classical IMS, it is still striking that HiKE-IMS shows significantly less spectral and chemical cross-sensitivities and thus exhibits considerably lower false-positive and false-negative rates. Overall, it thus turns out that HiKE-IMS is a promising alternative to classical IMS in the field of on-site detection of TICs.
Every drift tube ion mobility spectrometer (IMS) has an optimum drift voltage to reach maximum resolving power. This optimum depends, among other things, on the temporal and spatial width of the injected ion packet and the pressure within the IMS. A reduction of the spatial width of the injected ion packet leads to improved resolving power, higher peak amplitudes when operating the IMS at optimum resolving power, and thus a better signal-to-noise ratio despite the reduced number of injected ions. Hereby, the performance of electrospray ionization (ESI)-IMS can be considerably improved. By setting the ion shutter opening time to just 5 μs and slightly increasing the pressure, a high resolving power R P > 150 can be achieved with a given drift length of just 75 mm. At such high resolving power, even a mixture of the herbicides isoproturon and chlortoluron having similar ion mobility can be well separated despite short drift length.
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