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Register a new userProposal for the formation of ultracold deeply-bound RbSr dipolar molecules by all-optical methods
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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 textit{ab-initio} calculations, we analyze the feasibility of all-optical schemes for the formation of ultracold $^{87}$Rb$^{84}$Sr bosonic molecules. First, we have studied the formation by photoassociation followed by spontaneous emission. The photoassociation rates to levels belonging to electronic states converging to the $^{87}$Rb$(5s,^2S)$+$^{84}$Sr($5s5p,^3P_{0,1,2}$) asymptotes are particularly small close to the asymptote. The creation of molecules would be more interesting by using deeply levels that preferentially relaxes to the $v=0$ level of the ground state. On the other hands, the photoassociation rates to levels belonging to electronic states converging to the Rb$(5p,^2P_{1/2,3/2})$+Sr($5s^2,^1S$) asymptotes have high value close to the asymptote. The relaxation from the levels close to the asymptotes creates weakly-bound molecules in mosty only one vibrational level. Second, stimulated Raman adiabatic passage (STIRAP) achieved in a tight optical trap efficiently creates weakly-bound ground-state molecules in a well-defined level, thus providing an alternative to magnetic Feshbach resonances to implement several schemes for an adiabatic population transfer toward the lowest ground-state level of RbSr. Finally, we have studied STIRAP process for transferring the weakly-bound molecules into the $v=0$ level of the RbSr ground state.
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Recently, the quest for an ultracold and dense ensemble of polar molecules has attracted strong interest. Polar molecules have bright prospects for novel quantum gases with long-range and anisotropic interactions, for quantum information science, and for precision measurements. However, high-density clouds of ultracold polar molecules have so far not been produced. Here, we report a key step towards this goal. Starting from an ultracold dense gas of heteronuclear 40K-87Rb Feshbach molecules with typical binding energies of a few hundred kHz and a negligible dipole moment, we coherently transfer these molecules into a vibrational level of the ground-state molecular potential bound by >10 GHz. We thereby increase the binding energy and the expected dipole moment of the 40K-87Rb molecules by more than four orders of magnitude in a single transfer step. Starting with a single initial state prepared with Feshbach association, we achieve a transfer efficiency of 84%. While dipolar effects are not yet observable, the presented technique can be extended to access much more deeply bound vibrational levels and ultimately those exhibiting a significant dipole moment. The preparation of an ultracold quantum gas of polar molecules might therefore come within experimental reach.
We recently reported the formation of ultracold LiCs molecules in the rovibrational ground state X1Sigma+,v=0,J=0 [J. Deiglmayr et al., PRL 101, 133004 (2008)]. Here we discuss details of the experimental setup and present a thorough analysis of the photoassociation step including the photoassociation line shape. We predict the distribution of produced ground state molecules using accurate potential nergy curves combined with an ab-initio dipole transition moment and compare this prediction with experimental ionization spectra. Additionally we improve the value of the dissociation energy for the X1Sigma+ state by high resolution spectroscopy of the vibrational ground state.
We have studied the formation of ultracold RbSr molecules with laser pulses. After discussing the advantages of the Mott insulator phase for the control with pulses, we present two classes of strategies. The first class involves two electronic states. Two extensions of stimulated Raman adiabatic passage (STIRAP) for multi-level transitions are used : alternating STIRAP (A-STIRAP) and straddle STIRAP (S-STIRAP). Both transfer dynamics are modeled and compared. The second class of strategies involves only the electronic ground state and uses infrared (IR)/TeraHertz (THz) pulses. The chemical bond is first created by the application of a THz chirped pulse or $pi$-pulse. Subsequently, the molecules are transferred to their ro-vibrational ground state using IR pulses. For this last step, different optimized pulse sequences through optimal control techniques, have been studied. The relative merits of these strategies in terms of efficiency and robustness are discussed within the experimental feasibility criteria of present laser technology.
In this article we perform ab initio calculations in order to assess the reactivity of ultracold RbSr ($^2Sigma^+$) $+$ RbSr ($^2Sigma^+$) collisions occurring on the singlet as well as the triplet potential. At ultracold energies reactions are energetically possible if they release energy, i.e., they are exoergic. The exoergicity of reactions between RbSr molecules producing diatomic molecules are known experimentally. We extend this to reactions producing triatomic molecules by calculating the binding energy of the triatomic reaction products. We find that, in addition to the formation of Rb$_2$ and Rb$_2$+Sr$_2$ in singlet collisions, also the formation of Sr$_2$Rb and Rb$_2$Sr molecules in both singlet and triplet collisions is exoergic. Hence, the formation of these reaction products is energetically possible in ultracold collisions. For all exoergic reactions the exoergicity is larger than 1000 cm$^{-1}$. We also find barrierless qualitative reaction paths leading to the formation of the Rb$_2$Sr, Sr$_2$Rb, and singlet Rb$_2$ reaction products. These reaction paths imply the existence of a qualitative reaction path with a submerged barrier for the creation of the singlet Rb$_2$+Sr$_2$ reaction product. Because of the existence of these reactions we expect ultracold RbSr collisions to result in almost universal loss even on the triplet potential. Our results can be contrasted with collisions between alkali diatoms, where the formation of triatomic reaction products is endoergic, and with collisions between ultracold SrF molecules, where during triplet collisions only the spin-forbidden formation of singlet SrF$_2$ is allowed.
The formation of ultracold metastable RbCs molecules is observed in a double species magneto-optical trap through photoassociation below the ^85Rb(5S_1/2)+^133Cs(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.
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