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Concomitant species that appear at the same or very similar times in a mass-spectral analysis can clutter a spectrum because of the coexistence of many analyte-related ions (e.g., molecular ions, adducts, fragments). One method to extract ions stemming from the same origin is to exploit the chemical information encoded in the time domain, where the individual temporal appearances inside the complex structures of chronograms or chromatograms differ with respect to analytes. By grouping ions with very similar or identical time-domain structures, single-component mass spectra can be reconstructed, which are much easier to interpret and are library-searchable. While many other approaches address similar objectives through the Pearson’s correlation coefficient, we explore an alternative method based on a modified cross-correlation algorithm to compute a metric that describes the degree of similarity between features inside any two ion chronograms. Furthermore, an automatic workflow was devised to be capable of categorizing thousands of mass-spectral peaks into different groups within a few seconds. This approach was tested with direct mass-spectrometric analyses as well as with a simple, fast, and poorly resolved LC–MS analysis. Single-component mass spectra were extracted in both cases and were identified based on accurate mass and a mass-spectral library search.
New-found interest in the development of ionization sources for mass spectrometry, inspired by the advent of ambient desorption/ionization mass spectrometry, has led to a resurgence in plasma-source development and characterization. Dielectric-barrier discharges, particularly the low-temperature plasma (LTP) probe format, have been at the forefront of this field due to their low power consumption and relatively simple design. However, better fundamental understanding of this desorption/ionization source is needed to improve the analytical capabilities of such a device. Here, we use relatively fast (2.5 ms per spectrum) time-resolved mass spectrometry to characterize the temporal reagent-ion distribution from a low-frequency LTP probe. Different voltage waveforms were found to heavily influence the discharge properties and, consequently, ion production. Ion signals from short discharge pulses, ca. 40 µs, were found to be significantly broadened, ca. 10 ms, prior to extraction into the mass spectrometer. Additionally, higher frequencies of a sine-wave LTP produced the largest flux of reagent ions, which existed for most of the voltage waveforms. Finally, temporal signals for reagent and analyte ions were measured and related to specific ionization processes: proton transfer and charge transfer.