Studies are made of a system consisting of a molecule interacting with both an intense electromagnetic field resonant with a molecular transition frequency and a weak RF probe field at the Rabi frequency. An earlier study of this system (Freedhoff et al., ibid., vol.8, p.L209 (1975)) is extended to include the effects of photon cascades and of laser detuning. The method of calculation is the dressed-atom description and master-equation approach of Cohen-Tannoudji and Reynaud (1977). Unlike the earlier study, the present treatment produces quantitatively correct expressions for the emission and absorption spectra both in the visible and in the RF regions. More importantly, however, the predicted absorption intensity is greatly enhanced over that in the earlier study, and, for negative detuning of the laser, amplification of the RF signal is predicted.Studies are made of a system consisting of a molecule interacting with both an intense electromagnetic field resonant with a molecular transition frequency and a weak RF probe field at the Rabi frequency. An earlier study of this system (Freedhoff et al., ibid., vol.8, p.L209 (1975)) is extended to include the effects of photon cascades and of laser detuning. The method of calculation is the dressed-atom description and master-equation approach of Cohen-Tannoudji and Reynaud (1977). Unlike the earlier study, the present treatment produces quantitatively correct expressions for the emission and absorption spectra both in the visible and in the RF regions. More importantly, however, the predicted absorption intensity is greatly enhanced over that in the earlier study, and, for negative detuning of the laser, amplification of the RF signal is predicted.

Journal of Physics B Atomic and Molecular PhysicsMar 14, 197822 citations

Coherent Transient and Steady-State Phenomena in Coupled Molecular Transitions.

J. R. Rios Leite

Nov 1, 19771 citation

Induced and Spontaneous Emission in a Coherent Field. III

I. R. Senitzky

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.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.

Physical ReviewSep 15, 196019 citations

Coherent Stimulated Emission from Organic Molecular Crystals

Ernest G. Brock, P. Csavinszky, Ellis I. Hormats +3 more

The Journal of Chemical PhysicsAug 1, 196140 citations

Absorption and coherent emission of single molecules

Taras Plakhotnik

Journal of LuminescenceJul 1, 20027 citations

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.