3-PHOTON BIMOLECULAR ABSORPTION

Three-photon bimolecular absorption is a process which, through the simultaneous absorption of three laser photons, results in the electronic excitation of two molecules or atoms. Following a recent treatment of the selection rules, a quantum electrodynamical treatment is employed to describe the main features associated with the process and to produce an equation for the excitation rate. The dependence on photon polarization is investigated, and the magnitude of the excitation rate is estimated. It is shown that two different mechanisms operate, each with different selection rules and different dependences on intermolecular separation. In each case an energy mismatch is conveyed from one molecule to the other by means of virtual photon coupling. Some possible schemes for experimental study of the process are outlined.