Extracting Charge and Mass Information from Highly Congested Mass Spectra Using Fourier-Domain Harmonics

Journal of the American Society for Mass Spectrometry
Sean P ClearyJames S Prell

Abstract

Native mass spectra of large, polydisperse biomolecules with repeated subunits, such as lipoprotein Nanodiscs, can often be challenging to analyze by conventional methods. The presence of tens of closely spaced, overlapping peaks in these mass spectra can make charge state, total mass, or subunit mass determinations difficult to measure by traditional methods. Recently, we introduced a Fourier Transform-based algorithm that can be used to deconvolve highly congested mass spectra for polydisperse ion populations with repeated subunits and facilitate identification of the charge states, subunit mass, charge-state-specific, and total mass distributions present in the ion population. Here, we extend this method by investigating the advantages of using overtone peaks in the Fourier spectrum, particularly for mass spectra with low signal-to-noise and poor resolution. This method is illustrated for lipoprotein Nanodisc mass spectra acquired on three common platforms, including the first reported native mass spectrum of empty "large" Nanodiscs assembled with MSP1E3D1 and over 300 noncovalently associated lipids. It is shown that overtone peaks contain nearly identical stoichiometry and charge state information to fundamental peaks but ...Continue Reading

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Citations

Jan 9, 2019·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·Sean P Cleary, James S Prell
Apr 27, 2019·Journal of the American Society for Mass Spectrometry·Pavel I KitovJohn S Klassen
Apr 10, 2019·Journal of the American Society for Mass Spectrometry·Luis F SchachnerNeil L Kelleher
Oct 27, 2020·International Journal of Mass Spectrometry·Michael T Marty
Oct 30, 2020·Analytical Chemistry·James E KeenerMichael T Marty
Aug 21, 2021·Chemical Reviews·Sem TamaraAlbert J R Heck
Sep 3, 2021·Chemical Reviews·Amber D Rolland, James S Prell
Dec 17, 2021·Journal of the American Society for Mass Spectrometry·Andrew K SwansigerJames S Prell
Jan 15, 2022·Analytical Chemistry·Anthony M Pitts-McCoyScott A McLuckey

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