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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE

Single-molecule spectroscopy inside an optical cavity

Guangcun Shan, Shuying Bao, Wei Huang

Published Feb 13, 2006• 0 citations
Publisher

Abstract

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.

DOI
10.1117/12.676899

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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.
This work explores the feasibility of inducing lasing action in a single dye molecule using an optical microcavity. A single-molecule light source is proposed, in which a microcavity-coupled dye molecule is pumped by multiple energy donors via an intermolecular resonance energy transfer mechanism. A quantitative model based on realistic parameters for microcavities and for organic dyes shows that stimulated emission may become dominant over spontaneous fluorescence under optimal yet technically reachable conditions, suggesting the likelihood of achieving a single-molecule lasing photon source with the proposed device. Lasing of a single dye molecule generates signals much brighter than spontaneous fluorescence, and may find applications in a wide range of fields from physics and chemistry to biology.
Motivated by the recent progresses in one-atom laser and single-molecule manipulation, this work presents the model and simulations of a single dye molecule laser device, which consists of a single dye molecule as an acceptor in a microcavity pumped by multiple donors via the intermolecular resonance energy transfer mechanism. The photon intensity is calculated at the emission peaks of donor and acceptor dyes for different pump rates and donor numbers. Finally, it is demonstrated that stimulated emission gains a distinct advantage over spontaneous emission under appropriate conditions. This work would have many important applications in a wide range of fields from physics and chemistry to nanotechnology in future.
A significant limitation in the detection and spectroscopy of individual dye molecules in liquid room temperature samples is the loss of fluorescence signal through chromophore photobleaching. Although often considered a fundamental restriction on sensitivity, it has been shown that the probability per excitation cycle of photobleaching may be reduced by enhancing the spontaneous emission rate of the chromophore located inside a microdroplet, which acts as a optical cavity. Studies of glycerol microdroplets containing R6G dye molecules, and levitated in a three-dimensional electrodynamic trap, have demonstrated a significant enhancement of both the fluorescence decay rate [1] and the total fluorescence yield [2] of the chromophore. Modification of the emission rate is greatest for molecules located near the surface of small (< 10 μm) microdroplets, where the influence of the droplet cavity modes of the droplet is most significant. To exploit this surface sensitivity, surfactant forms of rhodamine dyes were recently studied [3]. Fluorescence emission of the dye molecules, constrained to the droplet surface and with fixed transition moments perpendicular to the surface normal, were shown to be significantly enhanced at small droplet sizes. Additionally, at larger droplet sizes corresponding to higher droplet Q’s, preferential emission into the cavity modes was observed, however the detection of fluorescence photons was delayed by the storage time of the cavity, which may be on the same order as the fluorescence lifetime. These measurements, performed on relatively concentrated dye solutions, suggest that microcavity effects may be exploited to greatly enhance single molecule detection sensitivity in glycerol microdroplets. Furthermore, the large cavity storage time of the high-Q droplets opens the possibility for re-excitation of the molecule following emission into the droplet resonance, and subsequent stimulated emission, that is, single-molecule lasing.
Optical cavity/molecule strong coupling offers attractive opportunities to modulate photochemical or photophysical processes. When atoms or molecules are placed in an optical cavity, they can coherently exchange photonic energy with optical cavity vacuum fields, entering the strong coupling interaction regime. Recent work suggests that the thermodynamic and kinetic properties of molecules can be significantly changed by strong coupling, resulting in the emergence of intriguing photochemical and photophysical phenomena. As more and more physico-chemical systems are studied under strong coupling conditions, optical cavities have also advanced in their sophistication, responsiveness, and (multi)functionality. In this review, we highlight some of these recent developments, particularly focusing on Fabry-Perot microcavities.
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.
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.