Olivier Dulieu

Ultracold Dipolar Molecules Composed of Strongly Magnetic Atoms.

In a combined experimental and theoretical effort, we demonstrate a novel type of dipolar system made of ultracold bosonic dipolar molecules with large magnetic dipole moments. Our dipolar molecules are formed in weakly bound Feshbach molecular states from a sample of strongly magnetic bosonic erbium atoms. We show that the ultracold magnetic molecules can carry very large dipole moments and we demonstrate how to create and characterize them, and how to change their orientation. Finally, we confirm that the relaxation rates of molecules in a quasi-two-dimensional geometry can be reduced by using the anisotropy of the dipole-dipole interaction and that this reduction follows a universal dipolar behavior.

Light-assisted cold chemical reactions of barium ions with rubidium atoms

Light-assisted reactive collisions between laser-cooled Ba+ ions and Rb atoms were studied in an ion–atom hybrid trap. The reaction rate was found to strongly depend on the electronic state of the reaction partners with the largest rate constant [7(2) × 10−11 cm3 s−1] obtained for the excited Ba+(6s)+Rb(5p) reaction channel. Similar to the previously studied Ca++Rb system, charge transfer and radiative association were found to be the dominant reactive processes. The generation of molecular ions by radiative association could directly be observed by their sympathetic cooling into a Coulomb crystal. Potential energy curves up to the Ba+(6s)+Rb(5p) asymptote and reactive-scattering cross sections for the radiative processes were calculated. The theoretical rate constant obtained for the lowest reaction channel Ba+(6s)+Rb(5s) is compatible with the experimental estimates obtained thus far.

Ion-neutral chemistry at ultralow energies: dynamics of reactive collisions between laser-cooled Ca+ ions and Rb atoms in an ion-atom hybrid trap

Cold chemical reactions between laser-cooled Ca+ ions and Rb atoms were studied in an ion-atom hybrid trap. Reaction rate constants were determined in the range of collision energies ⟨E coll⟩/k B=20 mK-20 K. The lowest energies were achieved in experiments using single localised Ca+ ions. Product branching ratios were studied using resonant-excitation mass spectrometry. The dynamics of the reactive processes in this system (non-radiative and radiative charge transfer as well as radiative association leading to the formation of CaRb+ molecular ions) have been analysed using high-level quantum-chemical calculations of the potential energy curves of CaRb+ and quantum-scattering calculations for the radiative channels. For the present low-energy scattering experiments, it is shown that the energy dependence of the reaction rate constants is governed by long-range interactions in line with the classical Langevin model, but their magnitude is determined by short-range non-adiabatic and radiative couplings which only weakly depend on the asymptotic energy. The quantum character of the collisions is predicted to manifest itself in the occurrence of narrow shape resonances at well-defined collision energies. The present results highlight both universal and system-specific phenomena in cold ion-neutral reactive collisions.

Anisotropic optical trapping of ultracold erbium atoms

Ultracold atoms confined in a dipole trap are submitted to a potential whose depth is proportional to the real part of their dynamic dipole polarizability. The atoms also experience photon scattering whose rate is proportional to the imaginary part of their dynamic dipole polarizability. In this article we calculate the complex dynamic dipole polarizability of ground-state erbium, a rare-earth atom that was recently Bose-condensed. The polarizability is calculated with the sum-over-state formula inherent to second-order perturbation theory. The summation is performed on transition energies and transition dipole moments from ground-state erbium, which are computed using the Racah-Slater least-square fitting procedure provided by the Cowan codes. This allows us to predict 9 unobserved odd-parity energy levels of total angular momentum J=5, 6 and 7, in the range 25000-31000 cm-1 above the ground state. Regarding the trapping potential, we find that ground-state erbium essentially behaves like a spherically-symmetric atom, in spite of its large electronic angular momentum. We also find a mostly isotropic van der Waals interaction between two ground-state erbium atoms, characterized by a coefficient C_6^{iso}=1760 a.u.. On the contrary, the photon-scattering rate shows a pronounced anisotropy, since it strongly depends on the polarization of the trapping light.

Formation of molecular ions by radiative association of cold trapped atoms and ions

Radiative emission during cold collisions between trapped laser-cooled Rb atoms and alkaline-earth ions (Ca+, Sr+, Ba+) and Yb+, and between Li and Yb+, are studied theoretically, using accurate effective core potential based quantum chemistry calculations of potential energy curves and transition dipole moments of the related molecular ions. Radiative association of molecular ions is predicted to occur for all systems with a cross section two to ten times larger than the radiative charge transfer one. Partial and total rate constants are also calculated and compared to available experiments. Narrow shape resonances are expected, which could be detectable at low temperature with an experimental resolution at the limit of the present standards. Vibrational distributions are also calculated, showing that the final molecular ions are not created in their ground state level.

Theory of Long-Range Ultracold Atom-Molecule Photoassociation.

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.

Long-range interactions between polar bialkali ground-state molecules in arbitrary vibrational levels

We have calculated the isotropic C6 coefficients characterizing the long-range van der Waals interaction between two identical heteronuclear alkali-metal diatomic molecules in the same arbitrary vibrational level of their ground electronic state X(1)Σ(+). We consider the ten species made up of (7)Li, (23)Na, (39)K, (87)Rb, and (133)Cs. Following our previous work [Lepers et al., Phys. Rev. A 88, 032709 (2013)], we use the sum-over-state formula inherent to the second-order perturbation theory, composed of the contributions from the transitions within the ground state levels, from the transition between ground-state and excited state levels, and from a crossed term. These calculations involve a combination of experimental and quantum-chemical data for potential energy curves and transition dipole moments. We also investigate the case where the two molecules are in different vibrational levels and we show that the Moelwyn-Hughes approximation is valid provided that it is applied for each of the three contributions to the sum-over-state formula. Our results are particularly relevant in the context of inelastic and reactive collisions between ultracold bialkali molecules in deeply bound or in Feshbach levels.

Long-range interactions between polar alkali-metal diatoms in external electric fields

We computed the long-range interactions between two identical polar bialkali molecules in their rovibronic ground level for all ten species involving Li, Na, K, Rb, and Cs, using accurate quantum chemistry results combined with available spectroscopic data. A huge van der Waals interaction is found for eight species in free space. The competition of the van der Waals interaction with the dipole-dipole interaction induced by an external electric field parallel or perpendicular to the intermolecular axis is investigated by varying the electric-field magnitude and the intermolecular distance. Our calculations predict a regime with the mutual orientation of the two molecules but with no preferential direction in the laboratory frame. A mechanism for the stimulated one-photon radiative association of a pair of ultracold polar molecules into ultracold tetramers is proposed, which would open the way towards the optical manipulation of ultracold polyatomic molecules.

Progress toward ultracold chemistry: ultracold atomic and photonic collisions

The dynamics of ultracold quantum gases composed of atoms or molecules with extremely low translational energy Et/kB << 1 millikelvin is dominated by the long-range mutual interactions between particles. Such studies require a detailed modelling of the atom-molecule or molecule-molecule long-range interactions inside the quantum gas with or without the presence of external fields. This paper focuses on two particular aspects relevant to ultracold chemistry: (i) The calculation of rates for photoassociation of a cold atom and a cold molecule to create ultracold excited trimers, based on the knowledge of the long-range interaction between the two species, showing that such rates are encouraging under the density and temperature conditions of a nearly degenerate quantum gas; (ii) The determination of the long-range interactions between two identical polar bialkali molecules in their rovibronic ground level in the presence of an electric field, showing the possibility for the formation of ultracold polar tetramers by stimulated emission.

Characterization of charge-exchange collisions between ultracold Li6 atoms and Ca40+ ions

We investigate the energy dependence and the internal-state dependence of the charge-exchange collision cross sections in a mixture of