Publication Date

5-2019

Department

Ames Laboratory; Chemistry

Campus Units

Ames Laboratory, Chemistry

OSTI ID+

1492061

Report Number

IS-J 9839

DOI

10.1111/php.13057

Journal Title

Photochemistry and Photobiology

Volume Number

95

Issue Number

3

First Page

773

Last Page

779

Abstract

The measurement of fluorescence lifetimes, especially in small sample volumes, presents the dual challenge of probing a small number of fluorophores and fitting the concomitant sparse data set to the appropriate excited‐state decay function. A common method of analysis, such as the maximum likelihood (ML) technique, assumes a uniform probability distribution of the parameters describing the fluorescence decay function. An improvement is thus suggested by implementing a suitable nonuniform distribution, as is provided by a Bayesian framework, where the distribution of parameters is obtained from both their prior knowledge and the evidence‐based likelihood of an event for a given set of parameters. We have also considered the Dirichlet prior distribution, whose mathematical form enables analytical solutions of the fitting parameters to be rapidly obtained. If Gaussian and exponential prior distributions are judiciously chosen, they reproduce the experimental target lifetime to within 20% with as few as 20 total photon counts for the data set, as does the Dirichlet prior distribution. But because of the analytical solutions afforded by the Dirichlet prior distribution, it is proposed to employ a Dirichlet prior to search parameter space rapidly to provide, if necessary, appropriate parameters for subsequent employment of a Gaussian or exponential prior distribution.

DOE Contract Number(s)

AC02-07CH11358

Language

en

Department of Energy Subject Categories

97 MATHEMATICS AND COMPUTING

Publisher

Iowa State University Digital Repository, Ames IA (United States)

Available for download on Friday, November 22, 2019

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