Title

Formation and analysis of ultracold polar molecules

Date of Completion

January 2007

Keywords

Physics, Molecular|Physics, Atomic

Degree

Ph.D.

Abstract

Alkali hydride molecules are polar, exhibiting large ground-state dipole moments. As ultracold sources of alkali atoms, as well as hydrogen, have been created in the laboratory, we explore theoretically the feasibility of forming such molecules from a mixture of the ultracold atomic gases, employing various photoassociation schemes. In this work we use lithium and sodium hydride as benchmark systems to calculate molecule formation rates through stimulated one-photon radiative association directly from the continuum as well as two-photon stimulated radiative association (Raman transfer) and excitation to bound levels of an excited state followed by spontaneous emission to the ground state. Using accurate molecular potential energy curves and dipole transition moments and with laser intensities and MOT densities that are easily attainable experimentally, we have found that substantial molecule formation rates can be realized even after the effect of back-stimulation has been accounted for. We examine the spontaneous emission cascade which takes place from the upper vibrational levels of the singlet ground state on a time scale of milliseconds. Because photon emission in the cascade process does not contribute to trap loss, a sizable population of molecules in the lowest vibrational level can be achieved. The triplet ground electronic state is of particular interest for experimental efforts since, although it has never been observed experimentally, molecular structure calculations of the a3Σ+ state for LiH and NaH predict a small van der Waals attraction, with a potential energy well so shallow that it can support only one bound rotational-vibrational level. Any molecule formed in the triplet ground state would then be immediately in the lowest and most stable level of that state and would be quite long-lived, unlike molecules in high vibrational levels which have significantly shorter lifetimes. As an analysis of our method of calculating molecule formation rates, we investigate more thoroughly the two-photon stimulated photoassociation process by employing the exact treatment of Dalgarno & Lewis to solve the Raman scattering problem. ^