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Importance of initial and final states as intermediate states in two‐photon spectroscopy of polar molecules
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4.Following the definition given in Ref. 5 we use the abbreviation “dipole forbidden” not only for transitions which are strictly forbidden by symmetry, but also for those for which the transition dipole moment is usually small due to the action of other less strict selection rules.
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15.After completion of this work (Ref. 16) an article by Martensen and Svendsen appeared in this journal (Ref. 17) in which a corresponding problem is discussed, with respect to Raman scattering. Here a similar confusion concerning initial and final states as intermediate states has been found in the literature. Since both Raman scattering and two‐photon absorption are two‐photon processes, the basic theoretical results of Martensen and Svendsen are similar to those derived in Sec. II. The final result, however, is quite different. In Raman scattering the neglect of initial and final states as intermediate states is (according to Martensen and Svendsen) of little importance, whereas, in two‐photon absorption these states may be responsible for the leading terms in the calculation of the cross section.
16.B. Dick, thesis, Universität du Köln, Köln, 1981.
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20.(a) H. H. Jaffé (private communication);
20.(b) P. Jaques, J. Faure, O. Chalvet, and H. H. Jaffé, J. Phys. Chem. 85, 473 (1981).
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