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Radiophysics and Quantum Electronics

Possible advantages of the excitation of stimulated two-photon emission in complex molecules

N. P. Bashlakova, Victor R. Blok, Yu. G. Khronopulo

Published Dec 1, 1985• 0 citations
Publisher
DOI
10.1007/bf01034165

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We investigate the feasibility of forming ultracold LiH from a mixture of the ultracold atomic gases, by using B 1 Π as an intermediate state in the photoassociation process. Using accurate molecular potential energy curves and dipole transition moments, we calculate and compare two possible schemes to populate vibrational levels of the ground electronic state, X 1 Σ + : (1) two-photon stimulated radiative association and (2) excitation to bound levels of the B 1 Π state, followed by spontaneous emission to the X 1 Σ + state. With laser intensities and atomic densities that are easily attainable experimentally, we find that significant quantities of molecules can be formed in various v , J levels of the electronic ground state. We examine the spontaneous emission cascade which takes place from the upper vibrational levels on a time scale of milliseconds. We discuss the issue of back-stimulation for the two-photon process and ways to mitigate it. Because photon emission in the cascade process does not contribute to trap loss, a sizable population of molecules in v = 0 can be achieved.
We describe recent results of experiments probing single molecules in the surface of spherical microcavities. Effects of spatial photoselection have been recently observed through changes in the single-molecule fluorescence photon statistics. In addition to being a sensitive probe of the highly interesting boundary region between classical and quantum mechanics, cavity-modified spontaneous emission and the possibility of single-molecule stimulated emission hold exciting promise as a means of exceeding sensitivity limitations such as photobleaching and absorption saturation in single molecule fluorescence detection. Ongoing efforts such as fluorescence imaging of single molecules on the surface of microspheres and attempts to observe single- molecule stimulated emission will also be described.