Four-Level Optical Line Shape of a Single Molecule Coupled to a Single Tunneling Two-Level System

Abstract

We propose a density-matrix theory for the four-level system consisting of a single optical two-level system (OTLS) coupled to a single two-level system tunneling along a vibrational coordinate (VTLS). Phonons induce jumping rates of the VTLS, but coherent tunneling has to be considered explicitly as well, because the Born-Oppenheimer potential of the tunnel variable may change upon optical excitation. The OTLS is subject to spontaneous emission and driven by a laser wave with arbitrary strength. Numerical simulations for various coupling cases reproduce limiting behaviors previously discussed separately in the literature, such as motional narrowing, cross transitions, optical saturation and pumping, and nonlinear effects. Our model also perfectly fits recent measurements of the spectra of a single molecule coupled to a single tunneling system in a disordered crystal.