Laser-induced resonance shifts of single molecules self-coupled by a metallic surface

Abstract

The spectral properties of single molecules placed near a metallic surface are investigated at low temperatures. Because of the high quality factor of the optical resonance, a laser-induced shift of the molecular lines is evidenced for the first time. The shift dependence on the laser excitation intensity and on the dephasing rate of the transition dipole is studied. A simple theoretical model of a laser-driven molecule self-coupled by a mirror is developed to qualitatively interpret the observations.