Molecular Spectroscopy with Coherent Radiation Sources

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Abstract
Various characteristics of molecules have been clarified by spectroscopic methods in which the interactions of molecules with the radiation field were investigated. A stationary response of a molecule excited by a radiation field appears as a spectral line. Information on molecules may be obtained from position (resonance frequency), intensity, and shape and width of the spectral line. So far the interaction of molecules with the radiation field has been studied primarily in a “frequency domain.” Although molecular spectroscopy is one of the research fields in modern science which has the longest history, a variety of important aspects have been demonstrated very recently in this field as radiation sources have been improved. When the radiation field is “weak,” the photon nature of the radiation field is dominant in the interaction with a molecule, such as in the cases of emission, absorption, and scattering of photons. When the radiation field is “strong,” in the sense that many photons exist in a proper mode of the radiation field, the wave nature of the field plays an important role in the interaction. In this case the radiation may be described in the form of the classical field, say, a sinusoidal function of the time and spatial coordinates, coherently interacting with the molecule, which is described quantum mechanically. Here nonlinear properties would appear in the interactions: saturation in absorption, induced scattering, multiphoton processes, coherent transients, etc.