Nanoscopic Charge Fluctuations in a Gallium Phosphide Waveguide Measured by Single Molecules

We present efficient evanescent coupling of single organic molecules to a gallium phosphide (GaP) subwavelength waveguide (nanoguide) decorated with microelectrodes. By monitoring their Stark shifts, we reveal that the coupled molecules experience fluctuating electric fields. We analyze the spectral dynamics of different molecules over a large range of optical powers in the nanoguide to show that these fluctuations are light-induced and local. A simple model is developed to explain our observations based on the optical activation of charges at an estimated mean density of 2.5×10^{22}  m^{-3} in the GaP nanostructure. Our work showcases the potential of organic molecules as nanoscopic sensors of the electric charge as well as the use of GaP nanostructures for integrated quantum photonics.