Fluctuations and single molecules

The fluorescence of single molecules coupled to a thermal bath is studied both experimentally and theoretically. The effect of different fluctuations on the coherence properties of resonance fluorescence is considered first. Coherence is measured in an interference experiment where a single molecule is used as a light source. A standard approach based on the optical Bloch equations apparently provides quite an accurate description of the interference experiment. Systems with long correlation times (where spectra are time dependent on any timescale) are considered next. It is shown that intensity-time-frequency correlation spectroscopy, which provides both high signal-to-noise ratio and high time resolution, is very suitable for such a case. The Bloch equations are further tested in an experiment where the shape of an excitation spectral line of a single molecule is accurately measured over six orders of magnitude of the exciting laser power. Significant deviations from the predictions of the Bloch equations are found. The role of critical parameters-the correlation time of the bath, the Rabi oscillation period, and the coupling constant between the bath and the molecule-is discussed. The paper also includes a short general introduction to the methodology of single-molecule studies.

Near-resonant holographic interferometry and absorption measurements of seeded atomic species in a flame

The development of near-resonant holographic interferometry techniques for use on flows seeded with atomic species is described. A theoretical model for the refractivity that is due to the seed species is outlined, and an approximation to this model is also described that is shown to be valid for practical regimes of interest and allows the number density of the species to be determined without knowledge of line-broadening effects. The details of quantitative number density experiments performed on an air-acetylene flame are given, and a comparison with an alternative absorption-based experiment is made. (C) 2004 Optical Society of America.