Kk. Sharman et al., Error analysis of the rapid lifetime determination method for double-exponential decays and new windowing schemes, ANALYT CHEM, 71(5), 1999, pp. 947-952
The rapid lifetime determination method (RLD) is a mathematical technique f
or extremely rapid evaluations of lifetimes in exponential decays, It has b
een applied in luminescence microscopy and single-molecule lifetime evaluat
ion. To date, the primary application has been in single-exponential evalua
tions. We present extensions of the method to double exponentials, Using Mo
nte Carlo simulations, we assess the performance of both the double-exponen
tial decay with known lifetimes and the double-exponential decay with unkno
wn preexponential factors and lifetimes. Precision is evaluated as a functi
on of the noise level (Poisson statistics), the ratios of the lifetimes, th
e ratios of their preexponential factors, and the fitting window. Optimum m
easurement conditions are determined. RLD is shown to work well over a wide
range of practical experimental conditions. If the lifetimes are known, th
e preexponential factors can be determined with good precision even at low
total counts (10(4)), With unknown preexponential factors and lifetimes, pr
ecisions decrease but are still acceptable. A new gating scheme (overlapped
gating) is shown to offer improved precision for the case of a single-expo
nential decay, Theoretical predictions are tested against actual experiment
al data from a laser-based lifetime instrument.