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Journal Article

Rapid deconvolution of low-resolution time-of-flight data using Bayesian inference

MPS-Authors
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Pieterse,  C. L.
Miller Group, Atomically Resolved Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;

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de Kock,  M.
Miller Group, Atomically Resolved Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Department of Physics, Stellenbosch University;

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Robertson,  W.
Miller Group, Atomically Resolved Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;

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Miller,  R. J. D.
Miller Group, Atomically Resolved Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Departments of Chemistry and Physics, University of Toronto;

Fulltext (public)

DECONPaperV7.pdf
(Preprint), 3MB

Supplementary Material (public)
Citation

Pieterse, C. L., de Kock, M., Robertson, W., Eggers, H. C., & Miller, R. J. D. (2019). Rapid deconvolution of low-resolution time-of-flight data using Bayesian inference. The Journal of Chemical Physics, 151(24): 244307. doi:10.1063/1.5129343.


Cite as: http://hdl.handle.net/21.11116/0000-0005-A273-2
Abstract
The deconvolution of low-resolution time-of-flight data has numerous advantages, including the ability to extract additional information from the experimental data. We augment the well-known Lucy-Richardson deconvolution algorithm using various Bayesian prior distributions and show that a prior of second-differences of the signal outperforms the standard Lucy-Richardson algorithm, accelerating the rate of convergence by more than a factor of four, while preserving the peak amplitude ratios of a similar fraction of the total peaks. A novel stopping criterion and boosting mechanism are implemented to ensure that these methods converge to a similar final entropy and local minima are avoided. Improvement by a factor of two in mass resolution allows more accurate quantification of the spectra. The general method is demonstrated in this paper through the deconvolution of fragmentation peaks of the 2,5-dihydroxybenzoic acid matrix and the benzyltriphenylphosphonium thermometer ion, following femtosecond ultraviolet laser desorption.