An experiment is described in which large numbers ( approximately 10 16 ) of calcium atoms are placed in the 4s4p 3 P metastable level by optical pumping with a tunable dye laser and then studied spectroscopically. Equations governing the degree of excitation by the laser are derived. Predictions of the theory are shown to be in good agreement with experimental results. In particular, at low optical depths produced by 10 15 ground state atoms cm -2 the dye laser raises approximately 50% of the calcium atoms into the metastable state. At higher optical depths associated with 10 17 ground state atoms cm -2 the number of excited states is limited only by the laser energy and line width. For the dye laser used the largest number of metastables produced was approximately 10 16 . The absorption spectra of the 4s4p 2 P level is seen out to 4s4p 3 P to 4s22d 3 D. The relaxation rate between the excited state fine structure is studied directly with an optically delayed dye laser continuum. Other applications of this technique of producing large numbers of excited states are briefly discussed.
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McIlrath et al. (1973) studied this question.
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