Abstract

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.

Highlights

  • 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

  • In 1973, Senitzky brought the controversy between vacuum fluctuations and radiation reaction to a satisfactory conclusion when he showed that their roles in spontaneous emission are “two sides of the same quantum-mechanical coin"

  • The end result is that the pump photon is annihilated, a Stokes photon is created, and the molecule has transitioned to the excited vibrational state. These results clearly show the advantage of the approach outlined above when the value of t increases beyond perturbative domains

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Summary

Results

The system is governed by an unperturbed , and a field Hamiltonian Ĥ F such that molecular

Raman interaction
The modified equations of motion for the fields are then
The polariton creation and annihilation operators obey the commutation relation
Discussion and conclusion
Additional information
Full Text
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