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

Abstract

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 ${\Gamma }_2=\frac{1}{2}{\Gamma }_1$ 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.

5 pages main text, 2 pages supplementary, 4 figures. Comments welcome

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