Orders of magnitude extension of the effective dynamic range of TDC-based TOFMS data through maximum likelihood estimation.

TitleOrders of magnitude extension of the effective dynamic range of TDC-based TOFMS data through maximum likelihood estimation.
Publication TypeJournal Article
Year of Publication2014
AuthorsIpsen A, Ebbels TMD
JournalJ Am Soc Mass Spectrom
Volume25
Issue10
Pagination1824-7
Date Published10/2014
ISSN1879-1123
KeywordsChromatography, Liquid, Likelihood Functions, Mass Spectrometry, Models, Theoretical
Abstract

In a recent article, we derived a probability distribution that was shown to closely approximate that of the data produced by liquid chromatography time-of-flight mass spectrometry (LC/TOFMS) instruments employing time-to-digital converters (TDCs) as part of their detection system. The approach of formulating detailed and highly accurate mathematical models of LC/MS data via probability distributions that are parameterized by quantities of analytical interest does not appear to have been fully explored before. However, we believe it could lead to a statistically rigorous framework for addressing many of the data analytical problems that arise in LC/MS studies. In this article, we present new procedures for correcting for TDC saturation using such an approach and demonstrate that there is potential for significant improvements in the effective dynamic range of TDC-based mass spectrometers, which could make them much more competitive with the alternative analog-to-digital converters (ADCs). The degree of improvement depends on our ability to generate mass and chromatographic peaks that conform to known mathematical functions and our ability to accurately describe the state of the detector dead time-tasks that may be best addressed through engineering efforts.

DOI10.1007/s13361-014-0961-5
Alternate JournalJ. Am. Soc. Mass Spectrom.
PubMed ID25049115
PubMed Central IDPMC4161928
Grant List080714/Z/06/Z / / Wellcome Trust / United Kingdom
MR/J013994/1 / / Medical Research Council / United Kingdom