We develop a theoretical description of photoassociative stimulated Raman adiabatic passage (STIRAP) near a Feshbach resonance in a thermal atomic gas. We show that it is possible to use low-intensity laser pulses to directly excite pairs of atoms in the continuum near a Feshbach resonance and to transfer most of the atomic cloud to the lowest rovibrational level of the molecular ground state. For a broad resonance, commonly found in several mixtures of alkali atoms, our model predicts a transfer efficiency up to 97% for a given atom pair, and up to 70% when averaged over an atomic ensemble. The laser intensities and pulse durations needed for such an optimal transfer, 10 2 –10 3 W cm −2 and several microseconds, are easily achievable experimentally. A single pair of STIRAP pulses converts an estimated fraction f ∼10 −6 –10 −4 of atoms in an atomic ensemble, leading to the production of 10–1000 molecules in a large sample of 10 7 atoms. A total of ∼10 4 –10 6 pulse pairs are thus required to transfer most atoms into molecules. Such an efficiency compares with or surpasses currently available techniques for creating stable diatomic molecules, and the versatility of this approach simplifies its potential use for many molecular species.
We develop a theoretical description of photoassociative stimulated Raman adiabatic passage (STIRAP) near a Feshbach resonance in a thermal atomic gas. We show that it is possible to use low-intensity laser pulses to directly excite pairs of atoms in the continuum near a Feshbach resonance and to transfer most of the atomic cloud to the lowest rovibrational level of the molecular ground state. For a broad resonance, commonly found in several mixtures of alkali atoms, our model predicts a transfer efficiency up to 97% for a given atom pair, and up to 70% when averaged over an atomic ensemble. The laser intensities and pulse durations needed for such an optimal transfer, 10 2 –10 3 W cm −2 and several microseconds, are easily achievable experimentally. A single pair of STIRAP pulses converts an estimated fraction f ∼10 −6 –10 −4 of atoms in an atomic ensemble, leading to the production of 10–1000 molecules in a large sample of 10 7 atoms. A total of ∼10 4 –10 6 pulse pairs are thus required to transfer most atoms into molecules. Such an efficiency compares with or surpasses currently available techniques for creating stable diatomic molecules, and the versatility of this approach simplifies its potential use for many molecular species.
One possibility for the creation of ultracold, high phase space density quantum gases of molecules in the rovibronic ground state relies on first associating weakly-bound molecules from quantum-degenerate atomic gases on a Feshbach resonance and then transferring the molecules via several steps of coherent two-photon stimulated Raman adiabatic passage (STIRAP) into the rovibronic ground state. Here, in ultracold samples of Cs2 Feshbach molecules produced out of ultracold samples of Cs atoms, we observe several optical transitions to deeply-bound rovibrational levels of the excited 0(u)+ molecular potentials with high resolution. At least one of these transitions, although rather weak, allows efficient STIRAP transfer into the deeply-bound vibrational level (see text for symbols)v = 73 > of the singlet X1 sigma(g)+ ground state potential, as recently demonstrated (J. G. Danzl, E. Haller, M. Gustavsson, M. J. Mark, R. Hart, N. Bouloufa, O. Dulieu, H. Ritsch, and H.-C. Nägerl, Science, 2008, 321, 1062). From this level, the rovibrational ground state (see text for symbols)v = 0, J = 0 > can be reached with one more transfer step. In total, our results show that coherent ground state transfer for Cs2 is possible using a maximum of two successive two-photon STIRAP processes or one single four-photon STIRAP process.
A quantum gas of ultracold molecules, with long-range and anisotropic interactions, will enable a series of fundamental studies in physics and chemistry. In particular, samples of ground-state molecules at ultralow temperatures and high number densities will facilitate the explorations of a large number of many-body physical phenomena and applications in quantum information processing. However, due to the lack of efficiently cooling techniques such as laser cooling for atomic gases, high number densities for ultracold molecular samples are not readily attainable. Associating ultracold atoms to weakly bound dimer molecules via Feshbach resonance and subsequently transferring them to a wanted molecular ro-vibronic ground state by a stimulated Raman adiabatic passages (STIRAP) have proved to be an effective way in producing ideal ultracold molecular samples. As a typical illustration, in a recent study (2010 Nat. Phys. 6 265) Danzl et al. experimentally realized the preparation of Cs2 molecule into its ro-vibronic ground state via two different multi-level STIRAPs:one is based on a single conversion route and the others are based on a cascade-connected route (labeled by 4p-STIRAP and s-STIRAP, respectively). In this work, we present a theoretical study for these two STIRAP schemes, focusing on the differences in physical principle and realistic performance between them. On the one hand, according to the theoretical approach of quasi-dark eigenstates, we conclude that a highly efficient population transfer is achievable in both schemes. On the other hand, by systematically studying the influences of the relevant parameters, including the spontaneous decays and the detunings from the intermediate states, and the temporal sequence and the amplitude of the laser pulses, we disclose their respective advantages and weaknesses in the realistic implementation. We theoretically predict that for both schemes their maximal conversion efficiencies each can attain 0.97 as long as the spontaneous decays from the intermediate excited states are sufficiently suppressed. Yet considering the fact that the already implemented efficiency is only around 0.6 for both schemes, there is still room for optimization, e.g. using stable Rydberg energy levels in future experiment. Furthermore, the success of these two schemes can provide a new route to the controllable entanglement preparation, opening more applications in the fields of quantum logic gate and so on.
We develop the theory for the Adiabatic Raman Photoassociation (ARPA) of ultracold atoms to form ultracold molecules in the presence of scattering resonances. Based on a computational method in which we replace the continuum with a discrete set of "effective modes", we show that the existence of resonances greatly aids in the formation of deeply bound molecular states. We illustrate our general theory by computationally studying the formation of 85Rb2 molecules from pairs of colliding ultracold 85Rb atoms. The single-event transfer yield is shown to have a near-unity value for wide resonances, while the ensemble-averaged transfer yield is shown to be higher for narrow resonances. The ARPA yields are compared with that of (the experimentally measured) "Feshbach molecule" magneto-association. Our findings suggest that an experimental investigation of ARPA at sub-μK temperatures is warranted.
We investigate theoretically the preparation of ultracold photoassociated Cs 2 molecules in the lowest vibrational level of the ground electronic state via the stimulated Raman adiabatic passage (STIRAP) by solving the time-dependent Schrödinger equation using the mapped Fourier grid method. A negative chirped laser pulse is used to produce the unstable photoassociated molecules in the excited electronic state. A dump pulse is utilized to transfer a partial population of the unstable photoassociated molecules to the vibrational v″ = 18 level of the ground electronic state. This part of population is then transferred to the v″ = 0 level of the ground electronic state by the pump and Stokes laser pulses via an intermediate state which is taken to be the v′ = 7 level of the excited electronic state, forming the stable photoassociated molecules. The population transfer efficiency from v″ = 18 to v″ = 0 in the ground electronic state reaches 96.2% via the STIRAP.
We report on the creation of ultracold (84)Sr(2) molecules in the electronic ground state. The molecules are formed from atom pairs on sites of an optical lattice using stimulated Raman adiabatic passage (STIRAP). We achieve a transfer efficiency of 30% and obtain 4×10(4) molecules with full control over the external and internal quantum state. STIRAP is performed near the narrow (1)S(0)-(3)P(1) intercombination transition, using a vibrational level of the 1(0(u)(+)) potential as an intermediate state. In preparation of our molecule association scheme, we have determined the binding energies of the last vibrational levels of the 1(0(u)(+)), 1(1(u)) excited-state and the X (1)Σ(g)(+) ground-state potentials. Our work overcomes the previous limitation of STIRAP schemes to systems with magnetic Feshbach resonances, thereby establishing a route that is applicable to many systems beyond alkali-metal dimers.
We suggest and analyze a technique for efficient and robust creation of dense ultracold molecular ensembles in their ground rovibrational state. In our approach a molecule is brought to the ground state through a series of intermediate vibrational states via a multistate chainwise stimulated Raman adiabatic passage technique. We study the influence of the intermediate states decay on the transfer process and suggest an approach that minimizes the population of these states, resulting in a maximal transfer efficiency. As an example, we analyze the formation of 87Rb2 starting from an initial Feshbach molecular state and taking into account major decay mechanisms due to inelastic atom-molecule and molecule-molecule collisions. Numerical analysis suggests a transfer efficiency >90, even in the presence of strong collisional relaxation as are present in a high density atomic gas.