Esposito Rosario, Mensitieri Giuseppe, de Nicola Sergio
Dept. of Chemical, Materials and Production Engineering, University of Naples Federico II, P.le Tecchio 80, 80125 Naples, Italy.
CNR-SPIN Napoli, Complesso Universitario di Monte Sant'Angelo, via Cinthia, 80126 Napoli, Italy.
Analyst. 2015 Dec 21;140(24):8138-47. doi: 10.1039/c5an01811k.
A new algorithm based on the Maximum Entropy Method (MEM) is proposed for recovering both the lifetime distribution and the zero-time shift from time-resolved fluorescence decay intensities. The developed algorithm allows the analysis of complex time decays through an iterative scheme based on entropy maximization and the Brent method to determine the minimum of the reduced chi-squared value as a function of the zero-time shift. The accuracy of this algorithm has been assessed through comparisons with simulated fluorescence decays both of multi-exponential and broad lifetime distributions for different values of the zero-time shift. The method is capable of recovering the zero-time shift with an accuracy greater than 0.2% over a time range of 2000 ps. The center and the width of the lifetime distributions are retrieved with relative discrepancies that are lower than 0.1% and 1% for the multi-exponential and continuous lifetime distributions, respectively. The MEM algorithm is experimentally validated by applying the method to fluorescence measurements of the time decays of the flavin adenine dinucleotide (FAD).
提出了一种基于最大熵方法(MEM)的新算法,用于从时间分辨荧光衰减强度中恢复寿命分布和零时间偏移。所开发的算法允许通过基于熵最大化的迭代方案和布伦特方法来分析复杂的时间衰减,以确定作为零时间偏移函数的约化卡方值的最小值。通过与不同零时间偏移值的多指数和宽寿命分布的模拟荧光衰减进行比较,评估了该算法的准确性。该方法能够在2000 ps的时间范围内以大于0.2%的精度恢复零时间偏移。对于多指数和连续寿命分布,寿命分布的中心和宽度的相对差异分别低于0.1%和1%。通过将该方法应用于黄素腺嘌呤二核苷酸(FAD)时间衰减的荧光测量,对MEM算法进行了实验验证。