Abstract
We have evaluated the use of two simple algorithms for determining the decay parameters describing a single exponential process for dyes with nanosecond and subnanosecond fluorescence lifetimes in the limit of low concentrations and high backgrounds from scattered photons generated by the solvent using experimental and Monte Carlo simulation results. These algorithms, the maximum likelihood estimator (MLE) and the rapid lifetime determination (RLD), are computationally easy to perform, allowing the evaluation of large amounts of data quickly and efficiently. The MLE and RLD methods were used to calculate the fluorescence lifetimes of three near-IR dyes with lifetimes spanning the range of 0.57 ns to 1.12 ns. For low-concentration conditions and high background-to-fluorescence ratios, the MLE method resulted in larger errors when compared to RLD, although both methods yielded comparable standard deviations. However, when the interval over which the lifetime was calculated within the decay profile was shifted to latter times in order to reduce the amount of scattered photons included in the calculation, significant improvements in the accuracy were observed with the use of MLE. Shifting the start channel of the calculation to latter time channels within the decay profile did not affect the lifetime with the use of RLD. Inclusion of large amounts of scattering photons was found to bias the calculated lifetime to lower values, reducing the accuracy of the determination. The relative standard deviations for MLE and RLD were found to be approximately 2–3% at a background-to-fluorescence ratio of 0.5. The absolute relative error in the methods at the 0.50 background-to-fluorescence ratio ranged from 14 to 27% for MLE and 8 to 18% for the RLD method when the calculation was initiated at t = 0. This error was found to decrease to < 1% with the use of MLE when the calculation was initiated at t ≈ 100 ps.
References
35
Referenced
26
10.1111/j.1751-1097.1984.tb03890.x
10.1021/j100325a044
10.1021/j100178a027
10.1021/ac00141a020
10.1063/1.1141885
10.1366/0003702914337182
10.1016/0301-4622(91)85036-P
10.1021/bi00240a024
10.1063/1.1142413
10.1021/ac00013a025
10.1364/JOSAB.9.001761
10.1063/1.109495
10.1016/0003-2697(74)90312-1
10.1098/rspa.1935.0076
10.1103/RevModPhys.25.818
10.1021/j150620a019
10.1366/0003702934048622
10.1021/ac00057a022
10.1021/ac00176a007
10.1021/ac00271a007
10.1021/ac00126a016
10.1021/ac00183a016
10.1366/0003702904417904
10.1021/ac00205a715
10.1016/0584-8539(90)80191-Z
10.1021/ac00006a716
10.1366/0003702914337119
10.1021/ac00024a024
10.1021/ac00031a004
10.1021/ac00053a019
10.1021/ac00042a009
- Mattingly Q. L. and Soper S. A, JACS, paper in press.
10.1016/0009-2614(90)85485-U
10.1021/ac00054a015
10.1073/pnas.86.11.4087
Dates
Type | When |
---|---|
Created | 15 years, 10 months ago (Oct. 14, 2009, 10:57 a.m.) |
Deposited | 5 months, 2 weeks ago (March 10, 2025, 12:36 p.m.) |
Indexed | 3 months ago (May 26, 2025, 4:24 p.m.) |
Issued | 31 years, 5 months ago (March 1, 1994) |
Published | 31 years, 5 months ago (March 1, 1994) |
Published Online | 31 years, 5 months ago (March 1, 1994) |
Published Print | 31 years, 5 months ago (March 1, 1994) |
@article{Soper_1994, title={Error Analysis of Simple Algorithms for Determining Fluorescence Lifetimes in Ultradilute Dye Solutions}, volume={48}, ISSN={1943-3530}, url={http://dx.doi.org/10.1366/0003702944028191}, DOI={10.1366/0003702944028191}, number={3}, journal={Applied Spectroscopy}, publisher={SAGE Publications}, author={Soper, Steven A. and Legendre, Benjamin L.}, year={1994}, month=mar, pages={400–405} }