Maximum entropy method for frequency-domain fluorescence lifetime analysis. 2. Timing, mismatched intensity, and reference lifetime errors.
Maximum entropy method for frequency-domain fluorescence lifetime analysis. 2. Timing, mismatched intensity, and reference lifetime errors.
复制标题
用于频域荧光寿命分析的最大熵方法。
DOI：
10.1021/ac950833l
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发表时间：
1996
影响因子：
7.4
通讯作者：
McGown,LB
中科院分区：
文献类型：
--
作者：
Shaver,JM;McGown,LB
最大熵法（MEM）通过同时最小化χ2拟合优度参数和最大化统计熵函数，使用广泛的衰减项拟合窗口，为荧光寿命数据提供了稳健和无偏的解决方案。本工作研究了频域测量中常见的三种系统误差对MEM荧光寿命恢复的影响。通过实际数据和模拟数据，将MEM恢复的系统误差在寿命分布中的表达式与标准非线性最小二乘（NLLS）分析进行了比较。随机噪声存在下的参考寿命误差对MEM和NLLS结果有相似的影响。恢复寿命、分数强度和峰形状的特征变化与真实参考寿命的识别有关。与NLLS相比，MEM在从包含时序或不匹配强度错误的数据中恢复寿命和分数强度方面提供了显着改进。这些改进与MEM的动态、自建模方法以及熵准则提供的方向有关。这些结果说明了最大熵方法在频域荧光寿命恢复以及其他应用中的效用。
The maximum entropy method (MEM) provides a robust and unbiased solution to fluorescence lifetime data through the use of a broad window of decay terms fit by simultaneous minimization of the χ2goodness-of-fit parameter and maximization of a statistical entropy function. This work investigated the effects of three systematic errors, common in frequency-domain measurements, on fluorescence lifetime recovery by MEM. Through real and simulated data, the expression of the systematic errors in lifetime distributions recovered by MEM was compared to that in standard nonlinear least-squares (NLLS) analysis. Reference lifetime errors in the presence of random noise had similar effects on both MEM and NLLS results. Characteristic changes in the recovered lifetimes, fractional intensities, and peak shapes were related to the identification of the true reference lifetime. Compared to NLLS, MEM afforded significant improvements for the recovery of lifetimes and fractional intensities from data containing timing or mismatched intensity errors. These improvements are linked to the dynamic, self-modeling approach of MEM and the direction provided by the entropy criterion. These results speak to the utility of the maximum entropy approach in frequency-domain fluorescence lifetime recovery as well as in other applications.