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Physical Review

Absorption and Collision Broadening of Resonance Radiation

Mark W. Zemansky

Published Nov 15, 1930• 0 citations
Publisher
DOI
10.1103/physrev.36.1591.2

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A radiative collision is a resonant energy transfer collision in which two atoms absorb or emit photons during the collision. Alternatively, a radiative collision is the emission or absorption of a photon from a transient molecule, and, as shown by Gallagher and Holstein, radiative collisions can also be described in terms of line broadening. In a line broadening experiment there are typically many atoms and weak radiation fields, and in a radiative collision experiment there are few atoms and intense radiation fields. The only real difference is whether there are many atoms or many photons. Due to the short collision times, ∼10 −12 s, simply observing radiative collisions between low lying states requires high optical powers, and entering the regime where the optical field is no longer a minor perturbation seems unlikely. Due to their long collision times and large dipole moments, Rydberg atoms provide the ideal system in which to study radiative collisions in a quantitative fashion. As we shall see, it is straightforward to enter the strong field regime in which the radiation field, a microwave or rf field to be precise, is no longer a minor perturbation. Ironically, while the experiments are radiative collision experiments, with few atoms and many photons, the description of the strong field regime is given in terms of dressed molecular states, which is more similar to a line broadening description.
The effect of collisions on the resonance fluorescence spectrum of two-level atoms excited by monochromatic resonance radiation is studied. Analysis is performed for systems where the Doppler broadening is small compared to the collision frequency (high buffer gas pressures) and for the general case where collisions arbitrarily change the phase of the radiation-induced dipole moment (from completely interrupted to completely unaffected phase of the dipole moment). Both at a relatively low and at a high excitation radiation intensity, the resonance fluorescence spectrum is shown to depend on whether the two-level system is closed or open. This is especially true for the narrow unshifted Rayleigh scattering line. It is shown that, although the absorption line is homogeneously broadened, the resonance fluorescence spectrum exhibits a clearly pronounced anisotropy. In a direction close to the direction of propagation of the excitation radiation, the Rayleigh scattering line is maximally narrowed. Under certain conditions (that can easily be created in experiments), the width of this line is proportional to the diffusion coefficient of atoms interacting with the radiation.