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Journal of Physics B Atomic Molecular and Optical Physics

Processes in the formation of ultracold NaCs

Christopher Haimberger, Jan Kleinert, Olivier Dulieu, N. P. Bigelow

Published Sep 25, 2006• 37 citations
Publisher

Abstract

The formation of electronic ground-state NaCs molecules from ultracold atoms by photoassociation is explored both experimentally and theoretically. We observe saturation of the photoassociation process as well as complete ionization of the molecular sample by resonant two-photon absorption. Measured absolute molecule formation rates are compared to theoretical calculations and shown to be in good agreement.

DOI
10.1088/0953-4075/39/19/s10

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The formation of electronic ground-state NaCs molecules from ultracold atoms by photoassociation is explored both experimentally and theoretically. We observe saturation of the photoassociation process as well as complete ionization of the molecular sample by resonant two-photon absorption. Measured absolute molecule formation rates are compared to theoretical calculations and shown to be in good agreement.
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The creation of ultracold molecules is currently limited to diatomic species. In this Letter, we present a theoretical description of the photoassociation of ultracold atoms and molecules to create ultracold excited triatomic molecules, thus being a novel example of a light-assisted ultracold chemical reaction. The calculation of the photoassociation rate of an ultracold Cs_{2} molecule in its rovibrational ground state with an ultracold Cs atom at frequencies close to its resonant excitation is reported, based on the solution of the quantum dynamics involving the atom-molecule long-range interactions and assuming a model potential for the short-range physics. The rate for the formation of excited Cs_{3} molecules is predicted to be comparable with currently observed atom-atom photoassociation rates. We formulate an experimental proposal to observe this process relying on the available techniques of optical lattices and standard photoassociation spectroscopy.
We demonstrate the direct formation of vibronic ground state RbCs molecules by photoassociation of ultracold atoms followed by radiative stabilization. The photoassociation proceeds through deeply bound levels of the (2)3Π0+ state. From analysis of the relevant free-to-bound and bound-to-bound Franck–Condon factors, we have predicted and experimentally verified a set of photoassociation resonances that lead to efficient creation of molecules in the v = 0 vibrational level of the X1Σ+ electronic ground state. We also compare the observed and calculated laser intensity required to saturate the photoassociation rate. We discuss the prospects for using short-range photoassociation to create and accumulate samples of ultracold polar molecules in their rovibronic ground state.
In this thesis properties of ultracold alkali dimers are studied both theoretically and experimentally. In the first, theoretical, part, the prospects for the formation of ultracold LiCs dimers in deeply bound vibrational levels using photoassociation (PA) are investigated. Furthermore a previous systematic investigation of the structure of all alkali dimers is extended by the ab initio calculation of static dipole polarizabilities. An extensive comparison with other published results supports the reliability of the chosen method. Based on these results an experimental scheme for the creation of an sample of oriented ultracold dipolar molecules is developed. In the second, experimental part the formation of LiCs ground state molecules by PA is investigated. PA spectroscopy is used to improve the accuracy of the potential energy curve for the B1P and the value of the dissociation energy of the X1S+ state significantly. The rovibrational distribution of ground state molecules is probed in a combination of resonance-enhanced multi-photon ionization and depletion spectroscopy. A simple scheme is found to form ultracold polar LiCs molecules in the absolute ground state X1S+,v''=0,J''=0. In a quasi-electrostatic trap created by a CO2 laser, LiCs molecules are formed and stored. A lifetime of 24(3)s, limited by collisions with background gas, is observed and rate coefficients for inelastic collisions between LiCs in high vibrational states and Cs atoms are determined. The long storage time facilitates the observation of radiative decay of polar molecules towards lower vibrational levels.
We describe the experimental observation of ultracold NaCs+{\mathrm{NaCs}}^{+}NaCs+ molecular formation in a novel two-species magneto-optical trap. We interpret our observations in terms of a photoassociative ionization pathway similar to that observed in a sodium trap: $\mathrm{Na}+\mathrm{Cs}+\ensuremath{\Elzxh}{\ensuremath{\omega}}_{\mathrm{Na}}+\ensuremath{\Elzxh}{\ensuremath{\omega}}_{\mathrm{Cs}}\ensuremath{\rightarrow}{\mathrm{NaCs}}^{+}{+e}^{\ensuremath{-}}$. We have directly measured the NaCs+{\mathrm{NaCs}}^{+}NaCs+ production rate as a function of the excitation laser frequency and intensity elucidating the role of ground-state hyperfine levels. We have observed resonance structures in the frequency-dependent ion rate which we associate with the molecular character of the process.
We present photoassociation spectroscopy of ultracold NaCs molecules formed in a dual-species magneto-optical trap. Excited-state molecules are formed in states correlating to the Na(3S 1/2 )+Cs(6P 3/2 ) asymptote. We assign the most prominent observed vibrational progression to the Ω=2 long range state based on a comparison with ab initio potentials. Molecules are secondarily excited before decaying to deeply bound levels of the electronic ground X 1 Σ + state where they are ionized and detected by time-of-flight mass spectroscopy.