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13 Continuous Formation of Vibronic Ground StateRbCs Molecules via Photoassociation

Colin Bruzewicz, Mattias Karl Gustavsson, Toshihiko Shimasaki

Published Aug 17, 2016• 47 citations
OpenAlex

Abstract

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.

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Formation of ultracold RbCs molecules by photoassociation

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The formation of ultracold metastable RbCs molecules is observed in a double species magneto-optical trap through photoassociation below the 85 Rb(5S 1/2 ) + 133 Cs(6P 3/2 ) dissociation limit followed by spontaneous emission. The molecules are detected by resonance enhanced two-photon ionization. Using accurate quantum chemistry calculations of the potential energy curves and transition dipole moment, we interpret the observed photoassociation process as occurring at short internuclear distance, in contrast with most previous cold atom photoassociation studies. The vibrational levels excited by photoassociation belong to the 5th 0 + or the 4th 0 − electronic states correlated to the Rb(5P 1/2, 3/2 ) + Cs(6S 1/2 ) dissociation limit. The computed vibrational distribution of the produced molecules shows that they are stabilized in deeply bound vibrational states of the lowest triplet state. We also predict that a noticeable fraction of molecules is produced in the lowest level of the electronic ground state.

arXiv:1111.3503•Laser Physics•Sep 3, 2012•23 citations
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.
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) 3 0 + 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 X 1 + 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.
We have produced ultracold, polar RbCs∗{\mathrm{R}\mathrm{b}\mathrm{C}\mathrm{s}}^{*}RbCs∗ molecules via photoassociation in a laser-cooled mixture of Rb and Cs atoms. Using a model of the RbCs∗{\mathrm{R}\mathrm{b}\mathrm{C}\mathrm{s}}^{*}RbCs∗ molecular interaction which reproduces the observed rovibrational structure, we infer decay rates in our experiments into deeply bound $X\text{ }^{1}\ensuremath{\Sigma}^{+}$ ground-state RbCs vibrational levels as high as $5\ifmmode\times\else\texttimes\fi{}{10}^{5}\text{ }{\mathrm{s}}^{\ensuremath{-}1}$ per level. Population in such deeply bound levels could be efficiently transferred to the vibrational ground state using a single stimulated Raman transition, opening the possibility to create large samples of stable, ultracold polar molecules.
Abstract We report the production of ultracold 85Rb133Cs molecules in their rovibronic ground state X 1Σ+ (v=0; J=0), by short‐range photoassociation (PA) to the 2 1Π1, 2 3Π1, and 3 3Σ states. In the PA frequency range from 11650 to 12150 cm−1 (corresponding to energy levels 15500–16000 cm−1 above the bottom of the X potential), we have observed 40 sets of new PA lines. For selected PA states, we investigate vibrational branching, rotational branching, and saturation behavior. Among these 40 new PA lines, the 3 3Σ (v=3) state has the highest molecule production rate of 2 x 103 molecules s−1 into the rovibronic ground state.
We have experimentally studied the formation of ultracold RbCs molecules by photoassociation at short internuclear range followed by spontaneous emission. The observation of new excited levels with respect to our previous work [Gabbanini and Dulieu, Phys. Chem. Chem. Phys. 13, 18905 (2011)] on both sides of the Rb(5S1/2)+Cs(6P3/2)\text{Rb}(5{S}_{1/2})+\text{Cs}(6{P}_{3/2})Rb(5S1/2​)+Cs(6P3/2​) dissociation limit gives information on the state responsible for molecule formation. The molecules are mainly formed in deeply bound levels of the electronic triplet ground state. The observed photoassociation transitions present differences in terms of saturation.
The formation of ultracold metastable RbCs molecules is observed in a double species magneto-optical trap through photoassociation below the 85 Rb(5S 1/2 ) + 133 Cs(6P 3/2 ) dissociation limit followed by spontaneous emission. The molecules are detected by resonance enhanced two-photon ionization. Using accurate quantum chemistry calculations of the potential energy curves and transition dipole moment, we interpret the observed photoassociation process as occurring at short internuclear distance, in contrast with most previous cold atom photoassociation studies. The vibrational levels excited by photoassociation belong to the 5th 0 + or the 4th 0 − electronic states correlated to the Rb(5P 1/2, 3/2 ) + Cs(6S 1/2 ) dissociation limit. The computed vibrational distribution of the produced molecules shows that they are stabilized in deeply bound vibrational states of the lowest triplet state. We also predict that a noticeable fraction of molecules is produced in the lowest level of the electronic ground state.