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Chinese Physics B

Profile function properties & optical transition formulae

Qingli Zhang, Guihua Sun, Jin-yun Gao, Dunlu L. Sun, Jianqiao Luo, Wenpeng Liu, Deming Zhang, Chaoshu Shi, Shaotang Yin

Published Jun 1, 2017• 1 citation
Publisher

Abstract

Profile function properties with different variables are discussed, the formulae of stimulated absorption, spontaneous and stimulated emission, absorption and emission coefficients, and cross sections are deduced, and some confusing issues are clarified.
DOI
10.1088/1674-1056/26/7/077803

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It is pointed out that the line profile coefficients for spontaneous and stimulated emission are identical in low-intensity radiation fields. In more intense radiation fields, however, the stimulated emission profiles in the radiative transfer equation and in the rate equations for the atomic level populations may differ from each other, owing to their different physical nature. A seeming discrepancy between the stimulated emission profiles of the usual semi-classical aproach and a recent quantum mechanical approach by Cooper et al. (1982), which should also be valid for intense 'broadband' fields, is discussed and shown to have negligible consequences for low-intensity radiation fields.
We present Einstein coefficient spectra and a detailed-balance derivation of generalized Einstein relations between them that is based on the connection between spontaneous and stimulated emission. If two broadened levels or bands overlap in energy, transitions between them need not be purely absorptive or emissive. Consequently, spontaneous emission can occur in both transition directions, and four Einstein coefficient spectra replace the three Einstein coefficients for a line. At equilibrium, the four different spectra obey five pairwise relationships and one lineshape generates all four. These relationships are independent of molecular quantum statistics and predict the Stokes' shift between forward and reverse transitions required by equilibrium with blackbody radiation. For Boltzmann statistics, the relative strengths of forward and reverse transitions depend on the formal chemical potential difference between the initial and final bands, which becomes the standard chemical potential difference for ideal solutes. The formal chemical potential of a band replaces both the energy and degeneracy of a quantum level. Like the energies of quantum levels, the formal chemical potentials of bands obey the Rydberg-Ritz combination principle. Each stimulated Einstein coefficient spectrum gives a frequency-dependent transition cross-section. Transition cross-sections obey causality and a detailed-balance condition with spontaneous emission, but do not directly obey generalized Einstein relations. Even with an energetic width much less than the photon energy, a predominantly absorptive forward transition with an energetic width much greater than the thermal energy can have such an extreme Stokes' shift that its reverse transition cross-section becomes predominantly absorptive rather than emissive.
A calculation is made of the stimulated emission threshold of organic dye solutions as a function of the diffusion coefficient, intensity of induced singlet–singlet or triplet–triplet absorption at the stimulated emission wavelength, steepness of the leading edge of pump pulses, and other parameters. It is shown that, if the dipole moment of a fluorescence transition is perpendicular to the dipole moments of associated induced singlet–singlet or triplet–triplet absorption transitions, the laser threshold of high–viscosity solutions is considerably lower than that of low-viscosity systems. The maximum value of the ratio of the cross sections of the singlet-singlet absorption and stimulated emission, at which a given molecule ceases to emit stimulated radiation, increases from 1 to 3 when the rotational diffusion coefficient decreases from ∞ to 0.