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Single dye molecules at cryogenic temperatures display many spectroscopicphenomena known from free atoms and are thus promising candidates forfundamental quantum optical studies. However, the existing techniques for thedetection of single molecules have either sacrificed the information on thecoherence of the excited state or have been inefficient. Here we show thatthese problems can be addressed by focusing the excitation light near to theabsorption cross section of a molecule. Our detection scheme allows us toexplore resonance fluorescence over 9 orders of magnitude of excitationintensity and to separate its coherent and incoherent parts. In the strongexcitation regime, we demonstrate the first observation of the Mollow tripletfrom a single solid-state emitter. Under weak excitation we report thedetection of a single molecule with an incident power as faint as 150 attoWatt,paving the way for studying nonlinear effects with only a few photons.

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