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arXiv:0809.4991 · Physical Review A

Efficient formation of deeply bound ultracold molecules probed by broadband detection

Matthieu Viteau, Amodsen Chotia, M. Allegrini, Nadia Bouloufa-Maafa, Olivier Dulieu, D. Comparat, P. Pillet

Published Feb 18, 2009• 29 citations
arXivHTMLPDF

Abstract

Using a nonselective broadband detection scheme we discovered an efficient mechanism of formation of ultracold ${\mathrm{Cs}}_{2}$ molecules in deeply bound vibrational levels $(v=1--9)$ of their electronic ground state $X\phantom{\rule{0.2em}{0ex}}^{1}\ensuremath{\Sigma}_{g}^{+}$. They are formed by a one-photon photoassociation of ultracold cesium atoms in a manifold of excited electronic states, followed by a two-step spontaneous emission cascade. This process creates about ${10}^{5}--{10}^{6}\phantom{\rule{0.3em}{0ex}}\text{molecules}\phantom{\rule{0.3em}{0ex}}\text{per}\phantom{\rule{0.3em}{0ex}}\text{second}$. This detection scheme is an advancement compare to previous ones and could be generalized to other molecular species for the systematic investigation of cold molecule formation mechanisms.

DOI
10.1103/physreva.79.021402

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Using a nonselective broadband detection scheme we discovered an efficient mechanism of formation of ultracold Cs2{\mathrm{Cs}}_{2}Cs2​ molecules in deeply bound vibrational levels (v=1−−9)(v=1--9)(v=1−−9) of their electronic ground state X1\ensuremathΣg+X\phantom{\rule{0.2em}{0ex}}^{1}\ensuremath{\Sigma}_{g}^{+}X1\ensuremathΣg+​. They are formed by a one-photon photoassociation of ultracold cesium atoms in a manifold of excited electronic states, followed by a two-step spontaneous emission cascade. This process creates about 105−−106moleculespersecond{10}^{5}--{10}^{6}\phantom{\rule{0.3em}{0ex}}\text{molecules}\phantom{\rule{0.3em}{0ex}}\text{per}\phantom{\rule{0.3em}{0ex}}\text{second}105−−106moleculespersecond. This detection scheme is an advancement compare to previous ones and could be generalized to other molecular species for the systematic investigation of cold molecule formation mechanisms.
By using broadband lasers, we demonstrate the possibilities for control of cold molecules formed via photoassociation. Firstly, we present a detection REMPI scheme (M. Viteau et al., Phys. Rev. A, 2009, 79, 021402) to systematically investigate the mechanisms of formation of ultracold Cs2 molecules in deeply bound levels of their electronic ground state X1sigma(g)+. This broadband detection scheme could be generalized to other molecular species. Then we report a vibrational cooling technique (M. Viteau et al., Science, 2008, 321, 232) through optical pumping obtained by using a shaped mode locked femtosecond laser. The broadband femtosecond laser excites the molecules electronically, leading to a redistribution of the vibrational population in the ground state via a few absorption-spontaneous emission cycles. By removing the laser frequencies corresponding to the excitation of the v = 0 level, we realize a dark state for the so-shaped femtosecond laser, leading, with the successive laser pulses, to an accumulation of the molecules in the v = 0 level, ie. a laser cooling of the vibration. The simulation of the vibrational laser cooling allows us to characterize the criteria to extend the mechanism to other molecular species (R. V. Krems, Int. Rev. Phys. Chem., 2005, 24, 99). We finally discuss the generalization of the technique to laser cooling of the rotation of the molecule.
We demonstrate the existence of a new mechanism for the formation of ultracold molecules via photoassociation of cold cesium atoms. The experimental results, interpreted with numerical calculations, suggest that a resonant coupling between vibrational levels of the 0+u (6s+6p1/2) and (6s+6p3/2) states enables formation of ultracold molecules in vibrational levels of the ground state well below the 6s+6s dissociation limit. Such a scheme should be observable with many other electronic states and atomic species.
Ultracold paramagnetic and polar diatomic molecules are among the promising systems for quantum simulation of lattice-spin models. Unfortunately, their experimental observation is still challenging. Based on our recent ab initio calculations, we analyze the feasibility of all-optical schemes for the formation of ultracold 87Rb84Sr^{87}\mathrm{Rb}^{84}\mathrm{Sr}87Rb84Sr bosonic molecules. A first possibility is photoassociation followed by spontaneous emission. The photoassociation rate coefficients toward electronic states converging to the 87Rb(5s2S1/2)+84Sr(5s5p3P0,1,2^{87}\mathrm{Rb}(5s\phantom{\rule{0.16em}{0ex}}^{2}S_{1/2})+^{84}\mathrm{Sr}(5s5p\phantom{\rule{0.16em}{0ex}}^{3}P_{0,1,2}87Rb(5s2S1/2​)+84Sr(5s5p3P0,1,2​) asymptotes are particularly small for vibrational levels close to the asymptote. The creation of molecules would be more interesting by using deeply bound levels which preferentially relax to the ${v}^{\ensuremath{'}\ensuremath{'}}=0$ level of the ground state. On the other hand, the photoassociation rate coefficients toward electronic states correlated to the Rb(5p2P1/2,3/2)+Sr(5s21S0\mathrm{Rb}(5p\phantom{\rule{0.16em}{0ex}}^{2}P_{1/2,3/2})+\mathrm{Sr}(5{s}^{2}\phantom{\rule{0.16em}{0ex}}^{1}S_{0}Rb(5p2P1/2,3/2​)+Sr(5s21S0​) are significant for levels close to the asymptote. The spontaneous emission thus creates weakly bound molecules in a single vibrational level. A second option relies on stimulated Raman adiabatic passage implemented in a tight optical trap. It efficiently creates weakly bound ground-state molecules in a well-defined level, thus providing a promising alternative to magnetic Feshbach resonances for further population transfer toward the absolute ground state of the RbSr molecule.
In recent years several groups of researchers have succeeded in making samples of cold molecules, at temperatures below 1 K, and of ultracold molecules, at temperatures below 1 mK. We concentrate on the formation of Cs2 dimers. Starting with laser-cooled atoms, photoassociation forms molecules in an excited electronic state. Various mechanisms are presented for stabilizing these molecules by spontaneous emission into a bound level of the ground electronic state. The design of new formation schemes requires precise knowledge of molecular potential curves that is well beyond the accuracy of ab initio calculations. We show that analytical long-range potentials can be fitted on photoassociation spectra and yield, through the determination of the C3 long-range coefficient, a value of the radiative lifetime of the 6P3/2 cesium level with an unprecedented accuracy. For short-range potentials it is possible to avoid explicit calculations by using asymptotic methods that generalize to long-range molecules the quantum-defect concepts developed for Rydberg atoms. Considering two coupled channels, we show how generalized Lu–Fano plots can extract precise information from experimental spectra.
The methods producing cold molecules from cold atoms tend to leave molecular ensembles with substantial residual internal energy. For instance, cesium molecules initially formed via photoassociation of cold cesium atoms are in several vibrational levels nu of the electronic ground state. We applied a broadband femtosecond laser that redistributes the vibrational population in the ground state via a few electronic excitation/spontaneous emission cycles. The laser pulses are shaped to remove the excitation frequency band of the nu = 0 level, preventing re-excitation from that state. We observed a fast and efficient accumulation ( approximately 70% of the initially detected molecules) in the lowest vibrational level, nu = 0, of the singlet electronic state. The validity of this incoherent depopulation pumping method is very general and opens exciting prospects for laser cooling and manipulation of molecules.
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.