By considering a radiating gas as a single quantum-mechanical system, energy levels corresponding to certain correlations between individual molecules are described. Spontaneous emission of radiation in a transition between two such levels leads to the emission of coherent radiation. The discussion is limited first to a gas of dimension small compared with a wavelength. Spontaneous radiation rates and natural line breadths are calculated. For a gas of large extent the effect of photon recoil momentum on coherence is calculated. The effect of a radiation pulse in exciting "super-radiant" states is discussed. The angular correlation between successive photons spontaneously emitted by a gas initially in thermal equilibrium is calculated.
We propose methods of optical pumping that are applicable to open, high-angular-momentum transitions in atoms and molecules, for which conventional optical pumping would lead to significant population loss. Instead of applying circularly polarized cw light, as in conventional optical pumping, we propose to use techniques for coherent population transfer (e.g., adiabatic fast passage) to arrange the atoms so as to increase the entropy removed from the system with each spontaneous decay from the upper state. This minimizes the number of spontaneous-emission events required to produce a stretched state, thus reducing the population loss due to decay to other states. To produce a stretched state in a manifold with angular momentum
J, conventional optical pumping requires about
2J spontaneous decays per atom; one of our proposed methods reduces this to about
log22J, while another of the methods reduces it to about one spontaneous decay, independent of
J.
We present a novel technique of efficient optical pumping of open, high-angular-momentum systems. The method combines two well-established approaches of population manipulation (conventional optical pumping and coherent population transfer), offering the ability to achieve higher population of a sublevel with the highest or lowest quantum number m (the “end state”) than obtainable with either of the techniques. To accomplish this task, we propose to use coherent-population-transfer technique (e.g., adiabatic fast passage) to arrange the system in such a way that spontaneously emitted photon (conventional optical pumping) carries away more entropy than in conventional schemes. This enables reduction of a number of spontaneous decays Nsd required to pump the system with the total angular momentum J from Nsd = J decays in the conventional scheme to Nsd ≲ log2(2J) decays in the proposed scheme. Since each spontaneous-emission event is potentially burdened with a loss of population (population is transferred to a dark state), this enables increasing population accumulated in the “end state”, which is important for many applications.