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Journal of the Optical Society of America B

Fluorescence correlation spectroscopy on a mirror

Hervé Rigneault, Pierre‐François Lenne

Published Oct 1, 2003• 22 citations
Publisher

Abstract

Fluorescence correlation spectroscopy when fluorescent nanoemitters are diffusing in the vicinity of a dielectric mirror is studied both theoretically and experimentally. We demonstrate that two important effects occur when the confocal detection volume is located on the mirror’s surface. First, the count rate per emitter is significantly enhanced owing to control of spontaneous emission and enhancement of the excitation field. Second, interference fringes in the excitation beam give rise to a new characteristic time in the photocurrent’s autocorrelation function. This new time is found to be independent of the transverse excitation field’s beam waist and permits accurate measurement of diffusion coefficients without any a priori knowledge of the confocal volume geometry.

DOI
10.1364/josab.20.002203

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Fluorescence correlation spectroscopy when fluorescent nanoemitters are diffusing in the vicinity of a dielectric mirror is studied both theoretically and experimentally. We demonstrate that two important effects occur when the confocal detection volume is located on the mirror’s surface. First, the count rate per emitter is significantly enhanced owing to control of spontaneous emission and enhancement of the excitation field. Second, interference fringes in the excitation beam give rise to a new characteristic time in the photocurrent’s autocorrelation function. This new time is found to be independent of the transverse excitation field’s beam waist and permits accurate measurement of diffusion coefficients without any a priori knowledge of the confocal volume geometry.
Summary form only given. Over the last three decades of the 20 th century many experiments have demonstrated that the rate of spontaneous emission for an emitter is determined by its electromagnetic surrounding. This phenomenon has been usually studied for atoms or molecules placed in the vicinity of mirrors or in optical resonators. Furthermore, it is also well-known that the fluorescence lifetime of an emitter changes after being embedded in dielectric media where aside from a change in the refractive index, it experiences the local fields in the dielectric. For a spherical medium larger than the order of a wavelength it is known that the coupling to Mie modes of this dielectric resonator has a large influence on the emission rate of an emitter inside. However, when the medium becomes comparable or smaller than a wavelength one can no longer speak of resonator modes. Here we report on an experiment where we have studied the variation of the spontaneous emission rate as the dielectric medium surrounding an emitter is made smaller and smaller down to a few nanometers.
Summary form only given. Over more than three decades many experiments have shown that the rate of spontaneous emission from an emitter can be strongly modified due to its electromagnetic surrounding. It is also well-known that the fluorescence lifetime of an emitter changes when embedded in dielectric media where aside from a change in the density of states, it is influenced by the local fields in the dielectric. The goal of our work has been to study the transition between the regime of an emitter in vacuum to that of a bulk dielectric medium, emphasizing the domain where the emitter's environment has a subwavelength extent. In our experiment we have investigated the dependence of the spontaneous emission rate of Eu/sup 3+/ ions in polymer nanospheres of different diameters, ranging from 20nm to 2000nm. In order to perform well-defined control experiments, we have combined atomic force microscopy and fluorescence confocal microscopy to make measurements only on isolated single spheres lying on a glass substrate.
Single-molecule fluorescence microscopy has been established in life science as an essential tool for studying the characteristics and dynamics of individual fluorescent emitters both in vitro as well as in vivo. Acquiring quantitative information from the confocal observation volume is still a challenging task and knowing the absolute number or concentration of proteins in, e.g., cellular structures can significantly improve our understanding of cell biology, which is an important step towards quantitative microscopy. In this talk, a new quantitative analytical tool called Counting by Photon Statistics (CoPS) will be presented. The approach relies on a statistical analysis of detected photon coincidences to estimate the number of independent fluorescent labels in the observation volume [1]. CoPS does exploit the photon antibunching effect: a single photon emitter can only generate one photon at a time. Originally developed for point measurements, CoPS has recently been extended to an imaging scheme [2]. Using a confocal fluorescence microscopy setup with pulsed excitation, four single-photon, detectors and parallellized time-correlated single photon counting electronics (MicroTime 200, PicoQuant), we prove the applicability of the method with artificial model systems (immobilized DNA origami) and present first steps towards biological samples. [1] Ta, H., Wolfrum, J., Herten, D.-P., An extended scheme for counting fluorescent molecules by photon-antibunching Laser Phys. 20:119 (2010). [2] Ta, H. et al., Mapping molecules in scanning far-field fluorescence nanoscopy. Nat. Commun. 6:7977 (2015).
Correlations between photons emitted by an atom in a laser field and near a metal surface are studied. With polarisation-dependent detection it is feasible to select photons which are emitted in a specific transition between degenerate substates. Both the Einstein coefficient for spontaneous decay of a particular excited substate and its branching towards the various ground states depend on the distance between the atom and the surface. A combination of these notions to design a geometry for the correlated detection of polarised photons is employed, in order to predict a strong dependence of the correlation functions on the atom-surface distance. In general, an enhancement of the correlations between emitted photons due to the presence of the metal surface is found if the atom-surface distance is (roughly) less than 20% of the wavelength of the fluorescence radiation. In particular the correlations between circularly polarised photons with the same helicity are modified dramatically, and the correlation time tends to infinity if the atom approaches the surface. It is pointed out how the different photon correlations can be understood from a simple interpretation of transition diagrams.
Resonance fluorescence of a two-level emitter displays persistently anti-bunching irrespective of the excitation intensity, but inherits the driving laser’s linewidth under weak monochromatic excitation. These properties are commonly explained in terms of two disjoined pictures, i.e., the emitter’s single photon saturation or passively scattering light. Here, we propose a unified model that treats all fluorescence photons as spontaneous emission, one at a time, and can explain simultaneously both the spectral and correlation properties of the emission. We theoretically derive the excitation power dependencies, measurable at the single-photon incidence level, of the first-order coherence of the whole resonance fluorescence and super-bunching of the spectrally filtered, followed by experimental confirmation on a semiconductor quantum dot micro-pillar device. Furthermore, our model explains peculiar coincidence bunching observed in phase-dependent two-photon interference experiments. Our work provides an intuitive understanding of coherent light-matter interaction and may stimulate new applications. Standard descriptions of resonance fluorescence consider either absorption and re-emission in a single-photon picture or passive scattering. This study shows that resonance fluorescence can be described by a pure quantum state of the emitter and photon, revealing a coherent superposition that challenges the conventional view of spontaneous emission as an incoherent process.