On-command enhancement of single molecule fluorescence using a gold nanoparticle as an optical nano-antenna

We investigate the coupling of a single molecule to a single spherical gold nanoparticle acting as a nano-antenna. Using scanning probe technology, we position the particle in front of the molecule with nanometer accuracy and measure a strong enhancement of more than 20 times in the fluorescence intensity simultaneous to a 20-fold shortening of the excited state lifetime. Direct comparison with three-dimensional calculations allow us to decipher the contributions of the excitation enhancement, spontaneous emission modification, and quenching. Furthermore, we provide direct evidence for the role of the particle plasmon resonance in the modification of the molecular emission.