A novel method for fast and robust estimation of fluorescence decay dynamics using constrained least-squares deconvolution with Laguerre expansion

We report a novel method for estimating fluorescence impulse response function (fIRF) from noise-corrupted time-domain fluorescence measurements of biological tissue. This method is based on the use of high-order Laguerre basis functions and a constrained least-squares approach that addresses the problem of overfitting due to increased model complexity. The new method was extensively evaluated on fluorescence data from simulation, fluorescent standard dyes, ex vivo tissue samples of atherosclerotic plaques and in vivo oral carcinoma. Current results demonstrate that this method allows for rapid and accurate deconvolution of multiple channel fluorescence decays without adaptively adjusting the Laguerre scale parameter. The appropriate choice of the scale parameter is essential for accurate estimation of the fIRF. The method described here is anticipated to play an important role in the development of computational techniques for real-time analysis of time-resolved fluorescence data from biological tissues and to support the advancement of fluorescence lifetime instrumentation for biomedical diagnostics by providing a means for on-line robust analysis of fluorescence decay.

[1]  Raluca Niesner,et al.  Noniterative biexponential fluorescence lifetime imaging in the investigation of cellular metabolism by means of NAD(P)H autofluorescence. , 2004, Chemphyschem : a European journal of chemical physics and physical chemistry.

[2]  Guy A. Dumont,et al.  Analysis of Flow Injection Peaks with Orthogonal Polynomials , 1994 .

[3]  Javier A. Jo,et al.  Automated Analysis of Fluorescence Lifetime Imaging Microscopy (FLIM) Data Based on the Laguerre Deconvolution Method , 2011, IEEE Transactions on Biomedical Engineering.

[4]  Qiyin Fang,et al.  Laguerre-based method for analysis of time-resolved fluorescence data: application to in-vivo characterization and diagnosis of atherosclerotic lesions. , 2006, Journal of biomedical optics.

[5]  Karsten König,et al.  Clinical multiphoton tomography and clinical two-photon microendoscopy , 2009, BiOS.

[6]  R. D. Dyson,et al.  Studies on the analysis of fluorescence decay data by the method of moments. , 1973, Biophysical journal.

[7]  Laura Marcu,et al.  Dynamic tissue analysis using time- and wavelength-resolved fluorescence spectroscopy for atherosclerosis diagnosis , 2011, Optics express.

[8]  N. Tanguy,et al.  Optimum choice of free parameter in orthonormal approximations , 1995, IEEE Trans. Autom. Control..

[9]  A. G. Szabo,et al.  The deconvolution of photoluminescence data , 1977 .

[10]  M A A Neil,et al.  Fluorescence lifetime imaging distinguishes basal cell carcinoma from surrounding uninvolved skin , 2008, The British journal of dermatology.

[11]  Qiyin Fang,et al.  Detection of rupture-prone atherosclerotic plaques by time-resolved laser-induced fluorescence spectroscopy. , 2009, Atherosclerosis.

[12]  M. Tachiya,et al.  Transient Effect in Fluorescence Quenching by Electron Transfer. 2. Determination of the Rate Parameters Involved in the Marcus Equation , 1995 .

[13]  Frank Y. S. Chuang,et al.  Fluorescence lifetime imaging microscopy: in vivo application to diagnosis of oral carcinoma. , 2009, Optics letters.

[14]  G. Dumont,et al.  An optimum time scale for discrete Laguerre network , 1993, IEEE Trans. Autom. Control..

[15]  Paritosh Pande,et al.  Fully automated deconvolution method for on-line analysis of time-resolved fluorescence spectroscopy data based on an iterative Laguerre expansion technique. , 2009, Journal of biomedical optics.

[16]  B. Valeur Analysis of time-dependent fluorescence experiments by the method of modulating functions with special attention to pulse fluorometry , 1978 .

[17]  B. Gallas,et al.  Sensitivity of Time-Resolved Fluorescence Analysis Methods for Disease Detection , 2010, IEEE Journal of Selected Topics in Quantum Electronics.

[18]  J. Siegel,et al.  Application of the stretched exponential function to fluorescence lifetime imaging. , 2001, Biophysical journal.

[19]  Laura Marcu,et al.  Multimodal characterization of compositional, structural and functional features of human atherosclerotic plaques , 2011, Biomedical optics express.

[20]  Anthony G. Constantinides,et al.  A novel algorithm for the adaptation of the pole of Laguerre filters , 2006, IEEE Signal Processing Letters.

[21]  V. Marmarelis Identification of nonlinear biological systems using laguerre expansions of kernels , 1993, Annals of Biomedical Engineering.

[22]  Y. Onganer,et al.  Fluorescence quenching of fluorescein with molecular oxygen in solution , 2005 .

[23]  William H. Press,et al.  Numerical Recipes: The Art of Scientific Computing , 1987 .

[24]  Sirajudeen Gulam Razul,et al.  Fluorescence lifetime discrimination using expectation-maximization algorithm with joint deconvolution. , 2009, Journal of biomedical optics.

[25]  Laura Marcu,et al.  Time-resolved fluorescence spectroscopy as a diagnostic technique of oral carcinoma: Validation in the hamster buccal pouch model. , 2010, Archives of otolaryngology--head & neck surgery.

[26]  Manoj Kumbhakar,et al.  Photophysical properties of coumarin-120: Unusual behavior in nonpolar solvents , 2003 .

[27]  W S Grundfest,et al.  Time-resolved Fluorescence Spectra of Arterial Fluorescent Compounds: Reconstruction with the Laguerre Expansion Technique , 2000, Photochemistry and photobiology.

[28]  E. Bakienė,et al.  Characterization of biological materials by frequency-domain fluorescence lifetime measurements using ultraviolet light-emitting diodes , 2008 .

[29]  P. French,et al.  Wide-field fluorescence lifetime imaging of cancer , 2010, Biomedical optics express.

[30]  H. Harry Asada,et al.  Laguerre-model blind system identification: cardiovascular dynamics estimated from multiple peripheral circulatory signals , 2005, IEEE Transactions on Biomedical Engineering.

[31]  William R. Ware,et al.  Deconvolution of fluorescence decay curves. A critical comparison of techniques , 1979 .

[32]  L. Brand,et al.  Analysis of fluorescence decay curves by means of the Laplace transformation. , 1975, Biophysical journal.

[33]  Qiyin Fang,et al.  Fast model-free deconvolution of fluorescence decay for analysis of biological systems. , 2004, Journal of biomedical optics.

[34]  R. Cubeddu,et al.  Time-resolved fluorescence imaging in biology and medicine , 2002 .

[35]  William R. Ware,et al.  Deconvolution of fluorescence and phosphorescence decay curves. Least-squares method , 1973 .

[36]  Laura Marcu,et al.  Development of a dual-modal tissue diagnostic system combining time-resolved fluorescence spectroscopy and ultrasonic backscatter microscopy. , 2009, The Review of scientific instruments.

[37]  J. Andre,et al.  Applications of fast Fourier transform to deconvolution in single photon counting , 1979 .

[38]  Kenneth T. V. Grattan,et al.  Prony’s method for exponential lifetime estimations in fluorescence‐based thermometers , 1996 .

[39]  B. Wahlberg,et al.  Modelling and Identification with Rational Orthogonal Basis Functions , 2000 .

[40]  T. Gabrecht,et al.  In vivo time-resolved spectroscopy of the human bronchial early cancer autofluorescence. , 2009, Journal of biomedical optics.

[41]  S. Druzhinin,et al.  Intramolecular Fluorescence Quenching of Crowned 7-Aminocoumarins as Potential Fluorescent Chemosensors , 2004, Journal of Fluorescence.