Quantum dynamics of a driven two-level molecule with variable dephasing

The longitudinal ($\Gamma_1$) and transverse ($\Gamma_2$) decay rates of a two-level quantum system have profound influence on its evolution. Atomic systems with $\Gamma_2=\tfrac{1}{2}\Gamma_1$ have been studied extensively, but with the rise of solid-state quantum devices it is also important to consider the effect of stronger transverse relaxation due to interactions with the solid environment. Here we study the quantum dynamics of a single organic dye molecule driven by a laser. We measure the variation of $\Gamma_2$ with temperature and determine the activation energy for thermal dephasing of the optical dipole. Then we measure the second-order correlation function $g^{(2)}(\tau)$ of the light emitted by the molecule for various ratios $\Gamma_2/\Gamma_1$ and saturation parameters $S$. We show that the general solution to the optical Bloch equations accurately describes the observed quantum dynamics over a wide range of these parameters, and we discuss the limitations of the various approximate expressions for $g^{(2)}(\tau)$ that appear in the literature.