Abstract
Stark effect modulation experiments were performed on single-molecule lines of terrylene in crystalline matrices of n-hexadecane and naphthalene at low temperatures. Modulation frequencies in the MHz range were used. The resulting fluorescence excitation spectra are distinctly different, depending on the relationship between the modulation frequency ω m and the molecular line width Γ. For ω m⪡ Γ, the single-molecule line exhibits a smooth broadening and apparent splitting into two components, whereas for ω m⪢ Γ it develops equidistant sidebands as in the case of phase modulation of an electromagnetic wave. It is further demonstrated that Stark effect modulation in the radio-frequency regime can be used to record absorption signals of single molecules with good signal-to-noise ratio.
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