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Journal of Lightwave Technology

Simple and Accurate Fluorescence Lifetime Measurement Scheme Using Traditional Time-Domain Spectroscopy and Modern Digital Signal Processing

Amirhassan Zareanborji, Huayong Yang, Graham E. Town, Yanhua Luo, Gang‐Ding Peng

Published Aug 25, 2016• 16 citations
Publisher

Abstract

Fluorescence lifetime measurement is an essential process for evaluation and application of optical gain media. An accurate and convenient scheme for fluorescence lifetime measurement of complex emission processes with either single or multiple fluorescence lifetimes is essential. We developed a new convolution-based scheme for fluorescence lifetime measurement. The innovation of the scheme lies in a combination of convolution-based digital signal processing algorithms with a low cost and simple time-domain spectroscopic setup. The convolution-based scheme is able to achieve accurate microsecond fluorescence lifetime resolution using the spectroscopic setup with only millisecond fluorescence lifetime resolution, for both single or multiple fluorescence lifetimes. We demonstrated the performance of the scheme, both theoretically and experimentally, by measuring fluorescence lifetimes associated with complicated emission processes in bismuth-erbium-doped fibers and erbium-doped fiber.

DOI
10.1109/jlt.2016.2603166

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Fluorescence lifetime measurement is an essential process for evaluation and application of optical gain media. An accurate and convenient scheme for fluorescence lifetime measurement of complex emission processes with either single or multiple fluorescence lifetimes is essential. We developed a new convolution-based scheme for fluorescence lifetime measurement. The innovation of the scheme lies in a combination of convolution-based digital signal processing algorithms with a low cost and simple time-domain spectroscopic setup. The convolution-based scheme is able to achieve accurate microsecond fluorescence lifetime resolution using the spectroscopic setup with only millisecond fluorescence lifetime resolution, for both single or multiple fluorescence lifetimes. We demonstrated the performance of the scheme, both theoretically and experimentally, by measuring fluorescence lifetimes associated with complicated emission processes in bismuth-erbium-doped fibers and erbium-doped fiber.
Many spectroscopic techniques today rely on time-resolved measurements under short excitation pulses. Instead of using a chopped pump excitation, or ultrafast optical pulses, we expand on and apply the previously developed set of frequency domain methods to analyze the population level dynamics in rare-earth-doped media. By identifying the full frequency response of the gain medium, this method can accurately yield excited state lifetimes and can also be used to estimate transition cross-sections. The accuracy of the frequency domain methods are verified with Er3+-and Tm3+-doped fibers, and an Al2O3:Tm3+waveguide, recovering similar results as reported by time-resolved techniques. The complete frequency domain model presented here can be used in characterization of novel optical gain media, and can provide insights into population dynamics in solid state amplifiers and lasers.
Classical time-resolved optical spectroscopy experiments are performed using sequences of ultrashort light pulses, with photon fluxes incident on the sample which are many orders of magnitude higher than real-world conditions corresponding to sunlight illumination. Spectroscopy and microscopy schemes that use quantum states of light have been widely described theoretically with fewer experimental demonstrations that typically require very long measurements that can extend for hours or more. Here, we show that time-resolved spectroscopy with quantum light can be performed without compromising measurement time or wavelength tunability, recording a fluorescence lifetime trace in biological samples in less than a second with acceptable signal-to-noise ratio. Starting from spontaneous parametric down-conversion driven by a continuous-wave laser, we exploit the temporal correlation between randomly generated signal/idler pairs to obtain temporal resolution, and their spectral correlation to select the excitation frequency. We also add spectral resolution in detection, using a 'photon-efficient' Fourier transform approach which employs a common-path interferometer. We demonstrate the potential of this approach by resolving, at the single-photon level, excitation energy transfer cascades from LH2 to LH1 in the photosynthetic membrane and disentangling the lifetimes of two dyes in a mixture. Our results provide a new approach to ultrafast optical spectroscopy, where experiments are performed under illumination intensity conditions comparable to real-world sunlight illumination.
A method for measuring the gain and the emission cross section of the four-level neodymium system in doped waveguides is presented. The method is based on a temporal analysis of the fluorescence decay occurring when the pump is switched off, after establishing a steady-state with high levels of absorbed power. For the case of doped fibers, results obtained using this method are compared with the usual low signal amplification technique, using a launched signal in the fiber, and the agreement is good. It is shown that the technique allows a rapid, simple method of determining low signal gain.>
Multiphoton fluorescence microscopy is now a well-established technique, currently attracting much interest across all fields of biophysics - especially with regard to enhanced focal resolution. The fundamental mechanism behind the technique, identified and understood through the application of quantum theory, reveals new optical polarization features that can be exploited to increase the information content of images from biological samples. In another development, based on a newly discovered, fundamentally related mechanism, it emerges the passage of off-resonant probe laser pulses may characteristically modify the intensity of single-photon fluorescence, and its associated optical polarization behavior. Here, the probe essentially confers optical nonlinearity on the decay transition, affording a means of optical control over the fluorescent emission. Compared to a catalogue of other laser-based techniques widely used in the life sciences, most suffer limitations reflecting the exploitation of specifically lifetime-associated features; the new optical control mechanism promises to be more generally applicable for the determination of kinetic data. Again, there is a prospect of improving spatial resolution, non-intrusively. It is anticipated that tight directionality can be imposed on single-photon fluorescence emission, expediting the development of new imaging applications. In addition, varying the optical frequency of the probe beam can add another dimension to the experimental parameter space. This affords a means of differentiating between molecular species with strongly overlapping fluorescence spectra, on the basis of their differential nonlinear optical properties. Such techniques significantly extend the scope and the precision of spatial and temporal information accessible from fluorescence studies.