Bayesian Deconvolution of Mass and Ion Mobility Spectra: From Binary Interactions to Polydisperse Ensembles

By M. Marty, A. Baldwin, E. Marklund, Georg K. A. Hochberg, J. Benesch, Carol V. Robinson. Analytical Chemistry, 2015

889 citations recorded by the source corpus.

Interpretation of mass spectra is challenging because they report a ratio of two physical quantities, mass and charge, which may each have multiple components that overlap in m/z. Previous approaches to disentangling the two have focused on peak assignment or fitting. However, the former struggle with complex spectra, and the latter are generally computationally intensive and may require substantial manual intervention. We propose a new data analysis approach that employs a Bayesian framework to separate the mass and charge dimensions. Based on this approach, we developed UniDec (Universal Deconvolution), software that provides a rapid, robust, and flexible deconvolution of mass spectra and ion mobility-mass spectra with minimal user intervention. Incorporation of the charge-state distribution in the Bayesian prior probabilities provides separation of the m/z spectrum into its physical mass and charge components. We have evaluated our approach using systems of increasing complexity, enabling us to deduce lipid binding to membrane proteins, to probe the dynamics of subunit exchange reactions, and to characterize polydispersity in both protein assemblies and lipoprotein Nanodiscs. The general utility of our approach will greatly facilitate analysis of ion mobility and mass spectra.

Subfields: Molecular Biology, Spectroscopy

View Paper: https://www.semanticscholar.org/paper/1403498a891d2ec041c16777dca70878ee3c1b86

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In Molecular Biology

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Citations in the corpus

• Boceprevir, GC-376, and calpain inhibitors II, XII inhibit SARS-CoV-2 viral replication by targeting the viral main protease (2020, positive): “Data were deconvolved and analyzed with UniDec.(41)”
• Generation of ordered protein assemblies using rigid three-body fusion (2020, positive): “…with Studier ’ s auto-induction (36) and purification, 2) oligomeric state determination by online buffer exchange mass spectrometry (37 – 41), 3) SAXS sample preparation and analytical tools for data collected at the Structurally Integrated Biology for Life Sciences (SIBYLS) Beamline…”
• Reconfigurable asymmetric protein assemblies through implicit negative design (2021, positive): “The recorded mass spectra were deconvolved with UniDec version 4.2+ ( 46 ).”