We extend the generating function technique for calculation of singlemolecule photon emission statistics [Y. Zheng and F. L. H. Brown, Phys. Rev.Lett., 90,238305 (2003)] to systems governed by multi-level quantum dynamics.This opens up the possibility to study phenomena that are outside the realm ofpurely stochastic and mixed quantum-stochastic models. In particular, thepresent methodology allows for calculation of photon statistics that arespectrally resolved and subject to quantum coherence. Several modelcalculations illustrate the generality of the technique and highlightquantitative and qualitative differences between quantum mechanical models andrelated stochastic approximations. Calculations suggest that studying photonstatistics as a function of photon frequency has the potential to reveal moreabout system dynamics than the usual broadband detection schemes.
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