Time-ordering in Heisenberg's equation of motion as related to spontaneous radiation.

Despite many years of research into Raman phenomena, the problem of how to include both spontaneous and stimulated Raman scattering into a unified set of partial differential equations persists. The issue is solved by formulating the quantum dynamics in the Heisenberg picture with a rigorous accounting for both time- and normal-ordering of the operators. It is shown how this can be done in a simple, straightforward way. Firstly, the technique is applied to a two-level Raman system, and comparison of analytical and numerical results verifies the approach. A connection to a fully time-dependent Langevin operator method is made for the spontaneous initiation of stimulated Raman scattering. Secondly, the technique is demonstrated for the much-studied two-level atom both in vacuum and in a lossy dielectric medium. It is shown to be fully consistent with accepted theories: using the rotating wave approximation, the Einstein A coefficient for the rate of spontaneous emission from a two-level atom can be derived in a manner parallel to the Weisskopf-Wigner approximation. The Lamb frequency shift is also calculated. It is shown throughout that field operators corresponding to spontaneous radiative terms do not commute with atomic/molecular operators. The approach may prove useful in many areas, including modeling the propagation of next-generation high-energy, high-intensity ultrafast laser pulses as well as spontaneous radiative processes in lossy media.