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Astrophysics and Space Science

Effects of an ambient medium on the emission, absorption and scattering of waves by atoms and molecules

D. B. Melrose

Published Jul 1, 1974• 3 citations
Publisher
DOI
10.1007/bf00642724

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Physical Review A•Nov 1, 1997•47 citations
Lasing refers to the generation of highly directional laser-like emission remotely pumped by laser pulses in a medium such as ambient air or a flame.It has been intensively investigated because of its potentials to revolutionize the field of remote sensing.Earlier studies were carried out in flames, where lasing effect has been observed in various radicals, for example H, O, N etc., through two-photon resonant excitation.This scheme was later applied to generate lasing of O and N in ambient air, which can be dramatically improved by predissociation of the air constituents.However, the underlying physical mechanism of two-photon-excited lasing effect is still unsettled although it has been studied for more than one decade.Currently there are three different proposals: (1) Amplified Spontaneous Emission (ASE), in which case population inversion is responsible for optical gain;(2) Superfluorescence (SF), where a macroscopic dipole occurs in the population inverted medium; (3) Both hyper-Raman scattering and four-wave mixing are involved in the generation of lasing emission.Here, we experimentally studied 656 nm lasing emission of atomic hydrogen via two-photon resonant excitation by focusing 125-fs laser pulses of 205-nm wavelength in a methane/oxygen welding flame (see Fig. 1), where hydrogen atoms are naturally present.Lasing occurs in both forward and backward directions, and the forward signal strength is almost one order of magnitude stronger than the backward one.It has been found that the durations of lasing pulses are around 20 ps, and decreases with increasing pump laser energies.Furthermore, the delay of the lasing pulse with respect to the pump pulse decreases with increasing pump energies.These results show high similarities with the behaviors of SF, suggesting that the femtosecond two-photonexcited lasing emission of atomic hydrogen might be SF.
We report on light amplification through stimulated emission in a dielectrically disordered medium. Liquid fragments confined in the solid matrix of porous quartz layers result in a random fluctuation of the dielectric function, and dye molecules embedded in the voids yield optical gain. The level of opacity is tunable by the ambient vapor pressure of the dielectric substance. In the multiple scattering regime, a strong intensity enhancement of the dye emission accompanied by significant spectral narrowing is observed above the threshold for a layer being in the opalescence state.
The decay rate of an excited molecule (atom) embedded in a dispersive and absorbing planar cavity is derived by using a recently obtained compact form of the Green's function for a multilayer. As a by-product, a hint is provided for a straightforward extension of the results obtained for lossless cavities of other shapes to the corresponding absorbing cavities. The decay rate in an absorbing cavity consists of the spontaneous emission rate and of the nonradiative rates caused by the near-field interaction of the molecule with the cavity medium and, for nearby molecules, with the cavity mirrors. Only the spontaneous emission rate is satisfactorily described in the macroscopic approach adopted. The theory is applied to an analysis of the effects of the weak cavity absorption on the decay rate in a dielectric microcavity formed by two metallic mirrors. As expected, dissipation in the cavity medium spoils the conditions for controlled spontaneuos emission and strongly suppresses the intensity of spontaneous emission. However, its effect on the spontaneous emission rate is much less pronounced.