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research article

Stochastic Approach to Data Analysis in Fluorescence Correlation Spectroscopy

Rao, R.  
•
Langoju, R.  
•
Gösch, M.
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2006
The Journal of Physical Chemistry A

Fluorescence correlation spectroscopy (FCS) has emerged as a powerful technique for measuring low concentrations of fluorescent molecules and their diffusion constants. In FCS, the experimental data is conventionally fit using standard local search techniques, for example, the Marquardt-Levenberg (ML) algorithm. A prerequisite for these categories of algorithms is the sound knowledge of the behavior of fit parameters and in most cases good initial guesses for accurate fitting, otherwise leading to fitting artifacts. For known fit models and with user experience about the behavior of fit parameters, these local search algorithms work extremely well. However, for heterogeneous systems or where automated data analysis is a prerequisite, there is a need to apply a procedure, which treats FCS data fitting as a black box and generates reliable fit parameters with accuracy for the chosen model in hand. We present a computational approach to analyze FCS data by means of a stochastic algorithm for global search called PGSL, an acronym for Probabilistic Global Search Lausanne. This algorithm does not require any initial guesses and does the fitting in terms of searching for solutions by global sampling. It is flexible as well as computationally faster at the same time for multiparameter evaluations. We present the performance study of PGSL for two-component with triplet fits. The statistical study and the goodness of fit criterion for PGSL are also presented. The robustness of PGSL on noisy experimental data for parameter estimation is also verified. We further extend the scope of PGSL by a hybrid analysis wherein the output of PGSL is fed as initial guesses to ML. Reliability studies show that PGSL and the hybrid combination of both perform better than ML for various thresholds of the mean- squared error (MSE).

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Type
research article
DOI
10.1021/jp055763t
Web of Science ID

WOS:000240496000004

Author(s)
Rao, R.  
Langoju, R.  
Gösch, M.
Rigler, P.
Serov, A.  
Lasser, T.  
Date Issued

2006

Published in
The Journal of Physical Chemistry A
Volume

110

Issue

37

Start page

10674

End page

10682

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
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Available on Infoscience
February 25, 2008
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/18985
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