Importance of initial and final states as intermediate states in two-photon spectroscopy of polar molecules

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Abstract
Two‐photon transitions may proceed via a mechanism not involving virtually excited intermediate states. For some examples, it is shown numerically that this mechanism may account for the largest contribution to the two‐photon cross section in polar molecules, if the dipole moment strongly alters with excitation. Possible consequences for the two‐photon detection of ’’forbidden’’ states in polar polyene systems are discussed.