Efficient coupling of photons to a single molecule and the observation of its resonance fluorescence

Abstract

Single dye molecules at cryogenic temperatures exhibit many spectroscopic phenomena known from the study of free atoms and are thus promising candidates for experiments in fundamental quantum optics. However, the existing techniques for their detection have either sacrificed information on the coherence of the excited state or have been inefficient. Here, we show that these problems can be addressed by focusing the excitation light near to the extinction cross-section of a molecule. Our detection scheme enables us to explore resonance fluorescence over nine orders of magnitude of excitation intensity and to separate its coherent and incoherent parts. In the strong excitation regime, we demonstrate the first direct observation of the Mollow fluorescence triplet from a single solid-state emitter. Under weak excitation, we report the detection of a single molecule with an incident power as faint as 600 aW, paving the way for studying nonlinear effects with only a few photons. © 2008 Nature Publishing Group.