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Quantum Electronics and Laser Science Conference

Photon correlation spectroscopy of Fluorescence Resonance Energy Transfer

Andrew J. Berglund, Andrew C. Doherty, Hideo Mabuchi

Published May 19, 2002• 0 citations
OpenAlex

Abstract

We report the use of a Hanbury-Brown Twiss apparatus to measure auto- and cross-correlations from pairs of dye molecules tethered to single strands of DNA and coupled by Fluorescence Resonance Energy Transfer (FRET). We observe non-classical photon anti-bunching, and we note that certain features of the observed correlations most likely arise from conformational fluctuations in the biomolecular substrate. These techniques should provide experimental access to molecular dynamics at nanosecond (and longer) timescales.

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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE•Feb 13, 2006•0 citations
We report the use of a Hanbury-Brown Twiss apparatus to measure auto- and cross-correlations from pairs of dye molecules tethered to single strands of DNA and coupled by Fluorescence Resonance Energy Transfer (FRET). We observe non-classical photon anti-bunching, and we note that certain features of the observed correlations most likely arise from conformational fluctuations in the biomolecular substrate. These techniques should provide experimental access to molecular dynamics at nanosecond (and longer) timescales.
We report high time-resolution measurements of photon statistics from pairs of dye molecules coupled by fluorescence resonance energy transfer (FRET). In addition to quantum-optical photon antibunching, we observe photon bunching on a time scale of several nanoseconds. We show by numerical simulation that configuration fluctuations in the coupled fluorophore system could account for minor deviations of our data from predictions of basic Förster theory. With further characterization we believe that FRET photon statistics could provide a unique tool for studying DNA mechanics on time scales from 10(-9)-10(-3) s.
The formation of protein complexes with other proteins and nucleic acids is critical to biological function. Although it is relatively easy to identify the components present in these complexes, it is often difficult to determine their exact stoichiometry and obtain information about the homogeneity of the sample from bulk measurements. We demonstrate the use of single molecule photon-pair correlation spectroscopy to distinguish between discrete numbers of molecules in biological complexes. Fluorescence photon antibunching is observed from a single molecule by employing time-correlated single photon counting in combination with a Hanbury-Brown and Twiss coincidence setup. In addition, pulsed laser excitation and time-tagged time-resolved data collection allow for the measurement of photon arrival times with nanosecond time resolution. The interphoton time distribution between consecutively arriving photons can be calculated and provides a measure of the second-order temporal correlation function. Analysis of this function yields an absolute measure of the number of molecules, N, present in a given complex. It is this ability to measure N that renders this technique powerful for determining stoichiometries in complex biological systems at the single molecule level. We investigate the counting efficiency and statistics of photon antibunching of specifically designed biological samples labeled with multiple copies of the same fluorescent dye and derive conclusions about its use in the analytical evaluation of complex biological samples.
For a single trapped ion, second-order time correlations of fluorescence photons are measured in a self-homodyne configuration by beating the fluorescence with itself. At the nanosecond timescale, the correlations are governed by electronic excitation and decay of the ion and anti-bunching in the resonance fluorescence is observed and quantitatively reproduced. On the other hand, at the microsecond timescale the motion of the ion determines the correlations: secular motional modes, their amplitude and relative coherence are measured. Besides precisely monitoring the trap frequencies, our observations also quantify the temporal stability of the trapping potential.
Antibunching is a quantum effect demonstrating clearly the quantum nature of the radiation field. Its detection through measurements of the second order correlation function is a direct proof of the presence of single molecule or single nano particle. In this paper we present the experimental setup of the Hanbury Brown - Twiss interferometer and the measurement results of the antibunching effect from single Rhodamine B dye molecules and single CdTe quantum dots in dilute solution. By fitting the second order correlation data, we derive a fluorescence lifetime of approximately 2 ns for Rhodamine B and 45 ns for CdTe quantum dots. Our results demonstrate an alternative way for determining the fluorescence lifetime using the antibunching effect.
Dynamic structural changes of macromolecules undergoing biochemical reactions can be studied using a novel single pair fluorescence resonance energy transfer (sp-FRET) tool which can be used as a nanoscale spectroscopic ruler. Although recent advances in applying such a nanoscale ruler to biological systems have been made, improvements in photon detectors and photophysical properties of the single FRET pair are still being studied. Motivated by the recent progresses in single-atom laser, we have investigated the ability to use the optical microcavity to amplify the sp-FRET signal. When the single FRET pair and the attached macromolecule of interest are placed inside an optical cavity with the emission mode of the acceptor dye in resonance with the cavity mode, quantitative modeling shows that, when adjusting the acceptor-cavity coupling parameters to be appropriate values, the acceptor fluorescence emission signal amplified by the cavity coupling mode would reach a significant value, leading to a much brighter sp-FRET spectroscopic signal. Possible applications to sp-FRET measurement of biological molecules are quantitatively examined.