Photon emission from driven single molecules

Abstract

The detection of photons emitted from a single molecule under the influence of electromagnetic radiation is considered. Utilizing a generating function formalism, we derive several exact results for the statistics of such emitted photons within the framework of the temporally modulated optical Bloch equations. Additionally, it is shown how these results reduce to previously obtained limiting behaviors. An appealing feature of this formulation is the inclusion of both photon bunching and anti-bunching effects within a single theoretical framework that is well suited for numerical analysis. Several examples are considered to demonstrate the feasibility of the approach in calculations. In most cases, these results verify known phenomena. In one case, we report a result that was missed by prior approximate treatments. This new effect centers around the fact that a chromophore will display anti-bunching behavior in the limit of fast modulation of the resonant absorption frequency.