Radiofrequency-optical double resonance spectroscopy

Meth. DR LA LM MB MW RA method of measurement applied to obtain the reported value double resonance experiments (microwave-optical double resonance MODR or radiofrequency-optical double resonance RFDR) Doppler free laser spectrosefipy laser magnetic resonance molecular beam electric resonance or molecular beam resonance with laser detection method microwave spectroscopy radio astronomy... 

When Brossel and Kastler proposed the intermarriage of optical spectroscopy and radiofrequency resonance nearly four decades ago, they triggered off the development of numerous novel spectroscopic methods— a development that continues even today. The first generation of optical pumping and optical double resonance experiments not only yielded a wealth of very precise data on atoms, molecules, condensed matter, and nuclei alike, but they also initiated the detailed study of the interaction of atoms with radiation, particularly under the aspects of coherence, and of the modification of atomic states through radiation fields. 

Laser-microwave spectroscopy based on nonlinear phenomena developed from the type of experiments on molecules already discussed in Section 3.2 which make use of optical pumping or double resonance. Occasionally, the laser and the rf power were high enough to create the nonlinear phenomena mentioned above, i.e., to saturate the transitions involved and/or to induce multiphoton transitions. The intermediate level in, e.g., two-photon transitions did not have to be a real state but could be virtual as well. Therefore, a drawback often encountered in earlier infared laser-microwave experiments could be avoided if the laser transition frequency did not exactly coincide with the molecular absorption line the Stark or Zeeman effect had to be used for tuning. This results in an undesired line splitting. With laser-microwave multiphoton processes, however, the laser can be operated at its inherent transition frequency. Exact resonance with molecular lines is then achieved by using a nonlinear effect, i.e., a radiofrequency quantum is added to or subtracted from the laser frequency (see Figure 28). 

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