aqora

In the previous articles of this series, dealing with the interaction between a number of molecules and the electromagnetic field in a resonant cavity, both the molecules and the field were treated by perturbation theory. The perturbation restriction on the field is removed in the present article, allowing large changes in the field, but the molecules are still assumed to undergo a small change during the time under consideration. The justification for this type of analysis, involving the generalization of the conventional concepts of induced and spontaneous emission, the applicability to a molecular amplifier during the buildup period, and the re-examination of a calculation by Serber and Townes concerning the fundamental limits of molecular amplification, is discussed.Two different molecular distributions are considered. In one (the resonant case) all molecules have the same frequency as the cavity, and in the other (the nonresonant case) there is a uniform frequency distribution. The molecules are assumed to be initially in an emissive state. Several types of driving fields are considered. Expressions are obtained for the field operators by the solution of a Volterra integral equation, and expectation values are obtained for the field strength and field energy.In the resonant case, both the coherent and incoherent fields increase exponentially after a sufficiently long time, no matter how small the initial gain is. Their ratio becomes constant and is equal to the number of photons in the driving field only in the absence of dissipation. An interesting related result is the fact that the signal-to-noise ratio for constant signal input power increases as the cavity dissipation increases. An estimate of the total time for which the theory is valid is obtained from a consideration of the energy emitted by the molecules. Contact is made with perturbation theory for sufficiently small gain and short time.In the nonresonant case the effect of the molecules is shown to be that of a negative dissipation. In contrast to the resonant case, the gain becomes exponential only if the negative dissipation exceeds, in absolute value, the true dissipation. The ratio of induced to spontaneous emission is, in this case also, equal to the number of photons in the driving field only in the absence of disipation. However, the signal-to-noise ratio for constant input power drops with increasing cavity dissipation.

The theory developed in the first two articles of this series, dealing with the interaction between the electromagnetic field in a cavity resonator and a number of two-level molecules, is generalized to include a Gaussian spread in the molecular frequency. The center of the molecular frequency distribution coincides with the cavity resonant frequency. There is a coherent driving field in the cavity at the same frequency, and cavity loss is taken into account.Using the formalism previously developed for a quantum-mechanical field in a lossy cavity, expressions are obtained by means of second-order perturbation theory for the expectation values of the field strength and field energy in the cavity, and of the power loss by the molecules. It is shown that the parts of the field energy resulting from induced and spontaneous emission, respectively, initially increase as the square of the time and approach steady-state values after (different, in general) transient periods, each of which is determined by two time constants: cavity relaxation time and inverse molecular frequency spread.It is also shown that both the induced and spontaneous emission power radiated by the molecules increase initially linearly with the time and approach steady-state values after transient periods. For the induced emission power, the transient period is determined by only one time constant, the inverse molecular frequency spread, while for the spontaneous emission power it is determined both by the inverse molecular frequency spread and the cavity relaxation time. The ratio of induced to spontaneous emission is initially

n

, and approaches a steady-state value $n{[\mathrm{exp}({r}^{2})(1\ensuremath{-}\mathrm{erf}r)]}^{\ensuremath{-}1},$ where

n

is the driving field energy in units of the photon energy, and

r

is the ratio of the cavity resonance width to molecular frequency spread. The seeming inconsistency of this value with the classical value of the ratio of the Einstein coefficients is discussed.