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Chemical Physics Letters

Theory of lineshapes in resonance scattering spectra

P. A. Hackett, R. A. Back

Published Jan 1, 1976• 9 citations
Publisher
DOI
10.1016/0009-2614(76)80228-x

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Lineshapes of three-level resonance Raman scattering and two-level resonance fluorescence, homogeneously broadened by collisions, in the presence of arbitrarily strong coherent radiation, are studied by means of a tetradic (density-matrix) scattering theory. In the case of medium coupling strength V L to the radiation field (where T 2 -1 <or=V L << tau c -1 , with T 2 and tau c being the coherence damping and collision times, respectively) the Mollow lineshape (1977) for resonance fluorescence is rederived, with proper T 2 and population cross-relaxation effects included. In particular it is shown that relaxation through intermediate non-resonant levels can considerably alter the lineshape in resonance fluorescence. In the case of strong coupling (V L >or approximately= tau c -1 ) the collision rates are modified by the applied field (optical collisions). It is shown that, whereas in self attenuation spectra optical collision rates can be obtained only from line intensity or line wing measurements, in resonance scattering these rates are directly obtained from linewidth measurements.