DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Photon Counting Data Analysis: Application of the Maximum Likelihood and Related Methods for the Determination of Lifetimes in Mixtures of Rose Bengal and Rhodamine B

Abstract

It is often convenient to know the minimum amount of data needed in order to obtain a result of desired accuracy and precision. It is a necessity in the case of subdiffraction-limited microscopies, such as stimulated emission depletion (STED) microscopy, owing to the limited sample volumes and the extreme sensitivity of the samples to photobleaching and photodamage. We present a detailed comparison of probability-based techniques (the maximum likelihood method and methods based on the binomial and the Poisson distributions) with residual minimization-based techniques for retrieving the fluorescence decay parameters for various two-fluorophore mixtures, as a function of the total number of photon counts, in time-correlated, single-photon counting experiments. The probability-based techniques proved to be the most robust (insensitive to initial values) in retrieving the target parameters and, in fact, performed equivalently to 2-3 significant figures. This is to be expected, as we demonstrate that the three methods are fundamentally related. Furthermore, methods based on the Poisson and binomial distributions have the desirable feature of providing a bin-by-bin analysis of a single fluorescence decay trace, which thus permits statistics to be acquired using only the one trace for not only the mean and median values of the fluorescence decay parameters butmore » also for the associated standard deviations. Lastly, these probability-based methods lend themselves well to the analysis of the sparse data sets that are encountered in subdiffraction-limited microscopies.« less

Authors:
 [1];  [1]; ORCiD logo [1]; ORCiD logo [1]
  1. Ames Lab. and Iowa State Univ., Ames, IA (United States). Dept. of Chemistry
Publication Date:
Research Org.:
Ames Lab., Ames, IA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1347904
Report Number(s):
IS-J-9225
Journal ID: ISSN 1089-5639
Grant/Contract Number:  
AC02-07CH11358; W-7405-430 ENG-82
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory
Additional Journal Information:
Journal Volume: 121; Journal Issue: 1; Journal ID: ISSN 1089-5639
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Santra, Kalyan, Smith, Emily A., Petrich, Jacob W., and Song, Xueyu. Photon Counting Data Analysis: Application of the Maximum Likelihood and Related Methods for the Determination of Lifetimes in Mixtures of Rose Bengal and Rhodamine B. United States: N. p., 2016. Web. doi:10.1021/acs.jpca.6b10728.
Santra, Kalyan, Smith, Emily A., Petrich, Jacob W., & Song, Xueyu. Photon Counting Data Analysis: Application of the Maximum Likelihood and Related Methods for the Determination of Lifetimes in Mixtures of Rose Bengal and Rhodamine B. United States. https://doi.org/10.1021/acs.jpca.6b10728
Santra, Kalyan, Smith, Emily A., Petrich, Jacob W., and Song, Xueyu. Mon . "Photon Counting Data Analysis: Application of the Maximum Likelihood and Related Methods for the Determination of Lifetimes in Mixtures of Rose Bengal and Rhodamine B". United States. https://doi.org/10.1021/acs.jpca.6b10728. https://www.osti.gov/servlets/purl/1347904.
@article{osti_1347904,
title = {Photon Counting Data Analysis: Application of the Maximum Likelihood and Related Methods for the Determination of Lifetimes in Mixtures of Rose Bengal and Rhodamine B},
author = {Santra, Kalyan and Smith, Emily A. and Petrich, Jacob W. and Song, Xueyu},
abstractNote = {It is often convenient to know the minimum amount of data needed in order to obtain a result of desired accuracy and precision. It is a necessity in the case of subdiffraction-limited microscopies, such as stimulated emission depletion (STED) microscopy, owing to the limited sample volumes and the extreme sensitivity of the samples to photobleaching and photodamage. We present a detailed comparison of probability-based techniques (the maximum likelihood method and methods based on the binomial and the Poisson distributions) with residual minimization-based techniques for retrieving the fluorescence decay parameters for various two-fluorophore mixtures, as a function of the total number of photon counts, in time-correlated, single-photon counting experiments. The probability-based techniques proved to be the most robust (insensitive to initial values) in retrieving the target parameters and, in fact, performed equivalently to 2-3 significant figures. This is to be expected, as we demonstrate that the three methods are fundamentally related. Furthermore, methods based on the Poisson and binomial distributions have the desirable feature of providing a bin-by-bin analysis of a single fluorescence decay trace, which thus permits statistics to be acquired using only the one trace for not only the mean and median values of the fluorescence decay parameters but also for the associated standard deviations. Lastly, these probability-based methods lend themselves well to the analysis of the sparse data sets that are encountered in subdiffraction-limited microscopies.},
doi = {10.1021/acs.jpca.6b10728},
journal = {Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory},
number = 1,
volume = 121,
place = {United States},
year = {Mon Dec 12 00:00:00 EST 2016},
month = {Mon Dec 12 00:00:00 EST 2016}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 6 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

The Number of Accumulated Photons and the Quality of Stimulated Emission Depletion Lifetime Images
journal, March 2014

  • Syed, Aleem; Lesoine, Michael D.; Bhattacharjee, Ujjal
  • Photochemistry and Photobiology
  • DOI: 10.1111/php.12248

Subdiffraction, Luminescence-Depletion Imaging of Isolated, Giant, CdSe/CdS Nanocrystal Quantum Dots
journal, February 2013

  • Lesoine, Michael D.; Bhattacharjee, Ujjal; Guo, Yijun
  • The Journal of Physical Chemistry C, Vol. 117, Issue 7
  • DOI: 10.1021/jp312231k

Supercontinuum Stimulated Emission Depletion Fluorescence Lifetime Imaging
journal, June 2012

  • Lesoine, Michael D.; Bose, Sayantan; Petrich, Jacob W.
  • The Journal of Physical Chemistry B, Vol. 116, Issue 27
  • DOI: 10.1021/jp303912p

Towards multi-exponential analysis in optically stimulated luminescence
journal, April 2010


Maximum likelihood method for the analysis of time-resolved fluorescence decay curves
journal, December 1991

  • Bajzer, ?eljko; Therneau, Terry M.; Sharp, Joseph C.
  • European Biophysics Journal, Vol. 20, Issue 5
  • DOI: 10.1007/BF00450560

Clarification of the use of CHI-square and likelihood functions in fits to histograms
journal, April 1984


Data analysis in the shot noise limit. 1. Single parameter estimation with Poisson and normal probability density functions
journal, November 1989


Data analysis in the shot noise limit. 2. Methods for data regression
journal, November 1989


On the analysis of fluorescence decay kinetics by the method of least-squares
journal, June 1974


Better estimates of exponential decay parameters
journal, October 1981

  • Hall, Peter; Selinger, Ben
  • The Journal of Physical Chemistry, Vol. 85, Issue 20
  • DOI: 10.1021/j150620a019

Comparison of maximum likelihood estimation and chi-square statistics applied to counting experiments
journal, January 2001

  • Hauschild, T.; Jentschel, M.
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 457, Issue 1-2
  • DOI: 10.1016/S0168-9002(00)00756-7

On the reliability of fluorescence decay data
journal, January 1977

  • Hinde, Al; Selinger, Bk; Nott, Pr
  • Australian Journal of Chemistry, Vol. 30, Issue 11
  • DOI: 10.1071/CH9772383

Single-Molecule Analysis And Lifetime Estimates Of Heterogeneous Low-Count-Rate Time-Correlated Fluorescence Data
journal, September 2011

  • Kim, Gi-Ho; Legresley, Sarah E.; Snyder, Nathaniel
  • Applied Spectroscopy, Vol. 65, Issue 9
  • DOI: 10.1366/10-06147

Efficient maximum likelihood estimator fitting of histograms
journal, May 2010


An Experimental Comparison of the Maximum Likelihood Estimation and Nonlinear Least-Squares Fluorescence Lifetime Analysis of Single Molecules
journal, May 2001

  • Maus, Michael; Cotlet, Mircea; Hofkens, Johan
  • Analytical Chemistry, Vol. 73, Issue 9
  • DOI: 10.1021/ac000877g

Comparison of Methods for Rapid Evaluation of Lifetimes of Exponential Decays
journal, May 2004


Artefacts in the analysis of temporal response functions measured by photon counting
journal, March 2005


Analysis of Fluorescence Decay by the Nonlinear Least Squares Method
journal, November 1988


Error Analysis of the Rapid Lifetime Determination Method for Double-Exponential Decays and New Windowing Schemes
journal, March 1999

  • Sharman, Kristin K.; Periasamy, Ammasi; Ashworth, Harry
  • Analytical Chemistry, Vol. 71, Issue 5
  • DOI: 10.1021/ac981050d

Analysis of fluorescence lifetime data for single Rhodamine molecules in flowing sample streams
journal, January 1994

  • Tellinghuisen, Joel.; Goodwin, Peter M.; Ambrose, W. Patrick.
  • Analytical Chemistry, Vol. 66, Issue 1
  • DOI: 10.1021/ac00073a013

Accurate Analysis of Fluorescence Decays from Single Molecules in Photon Counting Experiments
journal, August 2003

  • Turton, David A.; Reid, Gavin D.; Beddard, Godfrey S.
  • Analytical Chemistry, Vol. 75, Issue 16
  • DOI: 10.1021/ac034325k

Fluorescence Instrument Response Standards in Two-Photon Time-Resolved Spectroscopy
journal, August 2010


Testing Fluorescence Lifetime Standards using Two-Photon Excitation and Time-Domain Instrumentation: Rhodamine B, Coumarin 6 and Lucifer Yellow
journal, May 2014

  • Kristoffersen, Arne S.; Erga, Svein R.; Hamre, Børge
  • Journal of Fluorescence, Vol. 24, Issue 4
  • DOI: 10.1007/s10895-014-1368-1

The photophysics of rhodamine B
journal, January 1982


Photophysical properties of laser dyes: picosecond laser flash photolysis studies of Rhodamine 6G, Rhodamine B and Rhodamine 101
journal, January 1993

  • Beaumont, Paul C.; Johnson, David G.; Parsons, Barry J.
  • Journal of the Chemical Society, Faraday Transactions, Vol. 89, Issue 23
  • DOI: 10.1039/ft9938904185

Wavelength dependence of timing properties of the XP 2020 photomultiplier
journal, December 1978


Wavelength dependence of the time resolution of high-speed photomultipliers used in single-photon timing experiments
journal, January 1976


Systematic errors in χ2-fitting of Poisson distributions
journal, March 1996

  • Jading, Y.; Riisager, K.
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 372, Issue 1-2
  • DOI: 10.1016/0168-9002(95)01397-0

On the Use and Interpretation of Certain Test Criteria for Purposes of Statistical Inference: Part I
journal, July 1928

  • Neyman, J.; Pearson, E. S.
  • Biometrika, Vol. 20A, Issue 1/2
  • DOI: 10.2307/2331945

On the Use and Interpretation of Certain Test Criteria for Purposes of Statistical Inference: Part II
journal, December 1928

  • Neyman, J.; Pearson, E. S.
  • Biometrika, Vol. 20A, Issue 3/4
  • DOI: 10.2307/2332112

Works referencing / citing this record:

A Bayesian Approach for Extracting Fluorescence Lifetimes from Sparse Data Sets and Its Significance for Imaging Experiments
journal, December 2018

  • Santra, Kalyan; Smith, Emily A.; Song, Xueyu
  • Photochemistry and Photobiology, Vol. 95, Issue 3
  • DOI: 10.1111/php.13057

Coumarin‐based Fluorescent Probes for Selectively Targeting and Imaging the Endoplasmic Reticulum in Mammalian Cells
journal, August 2018

  • Wijesooriya, Chamari S.; Nieszala, Megan; Stafford, Alex
  • Photochemistry and Photobiology, Vol. 95, Issue 2
  • DOI: 10.1111/php.12985