Apodization Specific Fitting for Improved Resolution, Charge Measurement, and Data Analysis Speed in Charge Detection Mass Spectrometry

Miller, Zachary M.; Harper, Conner C.; Lee, Hyuncheol; Bischoff, Amanda J.; Francis, Matthew B.; Schaffer, David V.; Williams, Evan R.

doi:10.1021/jasms.2c00213

DOE OSTI · 1961825

Apodization Specific Fitting for Improved Resolution, Charge Measurement, and Data Analysis Speed in Charge Detection Mass Spectrometry

Miller, Zachary M.·Harper, Conner C.·Lee, Hyuncheol·Bischoff, Amanda J.·Francis, Matthew B.·Schaffer, David V.·Williams, Evan R.

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Abstract

Short-time Fourier transforms with short segment lengths are typically used to analyze single ion charge detection mass spectrometry (CDMS) data either to overcome effects of frequency shifts that may occur during the trapping period or to more precisely determine the time at which an ion changes mass or charge, or enters an unstable orbit. The short segment lengths can lead to scalloping loss unless a large number of zero-fills are used, making computational time a significant factor in real-time analysis of data. Apodization specific fitting leads to a 9-fold reduction in computation time compared to zero-filling to a similar extent of accuracy. This makes possible real-time data analysis using a standard desktop computer. Rectangular apodization leads to higher resolution than the more commonly used Gaussian or Hann apodization and makes it possible to separate ions with similar frequencies, a significant advantage for experiments in which the masses of many individual ions are measured simultaneously. Equally important is a >20% increase in S/N obtained with rectangular apodization compared to Gaussian or Hann, which directly translates to a corresponding improvement in accuracy of both charge measurements and ion energy measurements that rely on the amplitudes of the fundamental and harmonic frequencies. Finally, combined with computing the fast Fourier transform in a lower-level language, this fitting procedure eliminates computational barriers and should enable real-time processing of CDMS data on a laptop computer.

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Miller, Zachary M., Harper, Conner C., Lee, Hyuncheol, Bischoff, Amanda J., Francis, Matthew B., Schaffer, David V., Williams, Evan R.. 2022-09-29. Apodization Specific Fitting for Improved Resolution, Charge Measurement, and Data Analysis Speed in Charge Detection Mass Spectrometry. https://doi.org/10.1021/jasms.2c00213

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