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Abstract
Analysis of fluctuations in molecular fragmentation patterns reveals the structure and decomposition pathways of large, complex biomolecules.
Highlights
The spectroscopic study of the structure and dynamics of large polyatomic molecules poses a formidable experimental challenge, owing to spectral complexity and spectral congestion
We introduce a new method for the analysis of decompositions of large ionized molecules: twodimensional partial-covariance mass spectrometry. 2D-PCMS is based on a conceptually new idea of removing the nonphysical extrinsic correlations using the information contained in the acquired spectrum itself
The total ion count (TIC) parameter derived from the measured spectrum itself embodies the combined effect of all the known and unknown experimental parameters on each spectral signal simultaneously and serves as a key to unlocking the physical correlations between the biomolecular fragments within the self-correcting partialcovariance paradigm
Summary
The spectroscopic study of the structure and dynamics of large polyatomic molecules poses a formidable experimental challenge, owing to spectral complexity and spectral congestion. A solution to this challenge comes from multidimensional spectroscopic techniques, which reveal correlations between spectral signals, decongest the spectra, and provide supreme capabilities both for studying the mechanisms of molecular processes and for deducing. We develop a new type of two-dimensional (2D) partial-covariance spectroscopy applicable to fragmentations of large molecules, including polypeptide and full protein molecules well over 10 kilodaltons (kDa), thereby increasing the size of the systems amenable to covariance-mapping spectroscopy by 2 orders of magnitude. Contrary to the current state of the art, the new partial-covariance mapping extracts the spectral correlations using only the measured spectrum itself, without relying on any additional measurement channels
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