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The formation of Li$_2^+$ and subsequently Li$^+$ ions, during the excitation of $^7$Li atoms to the $3S_{1/2}$ state in a $^7$Li magneto optical trap (MOT), is probed in an ion-atom hybrid trap. Associative ionization occurs during the collision of Li($2P_{3/2}$) and Li($3S_{1/2}$) ultracold atoms, creating Li$_2^+$ ions. Photodissociation of Li$_2^+$ by the MOT lasers is an active channel for the conversion of Li$_2^+$ to Li$^+$. A fraction of the Li$_2^+$ ions is long lived even in the presence of MOT light. Additionally, rapid formation of Li$^+$ from Li$_2^+$ in the absence of MOT light is observed. Resonant excitation of ultracold atoms, resulting in intricate molecular dynamics, reveals important processes in ultracold dilute gases., Comment: The submitted manuscript consists of 10 pages including references. It consists of 11 figures including the figures in the supplemental material

Based on an accurate determination of the potential energy surfaces of Rb$_3^+$ correlated to its first asymptotic limit Rb$^+$$+$Rb($5s$)$+$Rb($5s$), we identify the presence of intersections of a pair of singlet and triplet surfaces over all interparticle distances, leading to Jahn-Teller couplings. We elaborate scenarios for charge exchange between ultracold charged atom-dimer complex (Rb$+$Rb$_2^+$ or Rb$^+$$+$Rb$_2$), predicting a strong selectivity on the preparation of the initial state of the dimer. We also demonstrate that the JT couplings must drive the three-body recombination (TBR) of Rb$^+$, Rb, and Rb at ultracold energies. Using the current analysis, we provide a consistent picture of the TBR experiments performed in ion-atom hybrid Rb samples \cite{dieterle2020inelastic,harter2012single}. We also demonstrate the presence of JT coupling as a general phenomenon in the singly-charged homonuclear alkali triatomic systems., Comment: 13 pages, 16 Figures

Hybrid atom-ion systems are a rich and powerful platform for studying chemical reactions, as they feature both excellent control over the electronic state preparation and readout as well as a versatile tunability over the scattering energy, ranging from the few-partial wave regime to the quantum regime. In this work, we make use of these excellent control knobs, and present a joint experimental and theoretical study of the collisions of a single $^{138}$Ba$^+$ ion prepared in the $5d\,^2D_{3/2,5/2}$ metastable states with a ground state $^6$Li gas near quantum degeneracy. We show that in contrast to previously reported atom-ion mixtures, several non-radiative processes, including charge exchange, excitation exchange and quenching, compete with each other due to the inherent complexity of the ion-atom molecular structure. We present a full quantum model based on high-level electronic structure calculations involving spin-orbit couplings. Results are in excellent agreement with observations, highlighting the strong coupling between the internal angular momenta and the mechanical rotation of the colliding pair, which is relevant in any other hybrid system composed of an alkali-metal atom and an alkaline-earth ion., Comment: 17 pages, 15 figures, 4 tables

We propose a method to engineer repulsive long-range interactions between ultracold ground-state molecules using optical fields, thus preventing short-range collisional losses. It maps the microwave coupling recently used for collisional shielding onto a two-photon transition, and takes advantage of optical control techniques. In contrast to one-photon optical shielding [Phys. Rev. Lett. 125, 153202 (2020)], this scheme avoids heating of the molecular gas due to photon scattering. The proposed protocol, exemplified for 23Na39K, should be applicable to a large class of polar diatomic molecules.

We theoretically investigate the collisional dynamics of laser-cooled $^{87}$Rb ground-state atoms and $^{40}$Ca$^+$ ground-state ions in the context of the hybrid trap experiment of Ref. [Phys. Rev. Lett. 107, 243202 (2011)], leading to ion losses. Cold $^{87}$Rb$^{40}$Ca$^+$ ground-state molecular ions are created by radiative association, and we demonstrate that they are protected against photodissociation by black-body radiation and by the $^{40}$Ca$^+$ cooling laser at 397~nm. This study yields an interpretation of the direct observation of $^{87}$Rb$^{40}$Ca$^+$ ions in the experiment, in contrast to other hybrid trap experiments using other species. Based on novel molecular data for the spin-orbit interaction, we also confirm that the non-radiative charge-exchange is the dominant loss process for Ca$^+$ and obtain rates in agreement with experimental observations and a previous calculation., Comment: PRA accepted. It includes 15 figures,29 pages, 45 references

Using the polarisation labelling spectroscopy, we performed the detailed analysis of the level structure of excited electronic states of the $^{39}$KCs molecule in the excitation energy interval between 17500~cm$^{-1}$ and 18600~cm$^{-1}$ above the $v=0$ level of the $X^1\Sigma^+$ ground state. We prove that the observed states are strongly coupled by spin-orbit interaction above 18200~cm$^{-1}$, as manifested by numerous perturbations in the recorded spectra. The spectra are interpreted with the guidance of accurate electronic structure calculations on KCs, including potential energy curves, transition electric dipole moments, and representation of the spin-orbit interaction with a quasi-diabatic effective Hamiltonian approach. The agreement between theory and experiment is found remarkable, clearly discriminating among the available theoretical data. This study confirms the accuracy of the polarisation labelling spectroscopy to analyse highly-excited electronic molecular states which present a dense level structure., Comment: 26 pages, 10 figures, laser spectroscopy, KCs molecules electronic states, potential energy curves, ab initio calculations

Ultracold temperatures in dilute quantum gases opened the way to an exquisite control of matter at the quantum level. Here we focus on the control of ultracold atomic collisions using a laser to engineer their interactions at large interatomic distances. We show that the entrance channel of two colliding ultracold atoms can be coupled to a repulsive collisional channel by the laser light so that the overall interaction between the two atoms becomes repulsive: this prevents them to come close together and to undergo inelastic processes, thus protecting the atomic gases from unwanted losses. We illustrate such an optical shielding mechanism with potassium and cesium atoms colliding at ultracold temperature (\textless 1 microkelvin). The process is described in the framework of the dressed-state picture and we then solve the resulting staionary coupled Schr\"{o}dinger equations. The role of spontaneous emission and photoinduced inelastic scattering is also investigated as possible limitations of the shielding efficiency. We predict an almost complete suppression of inelastic collisions using a laser-induced coupling characterized by a Rabi frequency of $\omega = 200$~MHz and a frequency detuned from the potassium D2 transition by $\Delta = 200$~MHz. We found the polarization of the laser has no influence on this efficiency. This proposal could easily be formulated for other bi-alkali-metal pairs as their long-range interaction are all very similar to each other.

Starting from an ultracold sample of ground-state $^{23}$Na$^{87}$Rb molecules, we investigate the lowest ro-vibrational level of the $b^3\Pi$ state with high resolution laser spectroscopy. This electronic spin-forbidden $X^1\Sigma^+ \leftrightarrow b^3\Pi$ transition features a nearly diagonal Franck-Condon factor and has been proposed useful for probing and manipulating the ultracold molecular gas. We measure the transition strength directly by probing the ac Stark shift induced by near resonance light and determine the total excited-state spontaneous emission rate by observing the loss of molecules. From the extracted branching ratio and the theoretical modeling, we find that the leakage to the continuum of the $a^3\Sigma^+$ state plays the dominant role in the total transition linewidth. Based on these results, we show that it is feasible to create optical trapping potentials for maximizing the rotational coherence with laser light tuned to near this transition., Comment: 8 pages, 5 figures

We propose a method to suppress the chemical reactions between ultracold bosonic ground-state $^{23}$Na$^{87}$Rb molecules based on optical shielding. By applying a laser with a frequency blue-detuned from the transition between the lowest rovibrational level of the electronic ground state $X^1\Sigma^+ (v_X=0, j_X=0)$, and the long-lived excited level $b^3\Pi_0 (v_b=0, j_b=1)$, the long-range dipole-dipole interaction between the colliding molecules can be engineered, leading to a dramatic suppression of reactive and photoinduced inelastic collisions, for both linear and circular laser polarizations. We demonstrate that the spontaneous emission from $b^3\Pi_0 (v_b=0, j_b=1)$ does not deteriorate the shielding process. This opens the possibility for a strong increase of the lifetime of cold molecule traps, and for an efficient evaporative cooling. We also anticipate that the proposed mechanism is valid for alkali-metal diatomics with sufficiently large dipole-dipole interactions.

We calculate the isotope independent Li$^+$-Li potential energy curves for the electronic ground and first excited states. Scattering phase shifts and total scattering cross section for the $^7$Li$^+$-$^7$Li collision are calculated with emphasis on the ultra-low energy domain down to the $s$-wave regime. The effect of physically motivated alterations on the calculated potential energy curves is used to determine the bound of accuracy of the low-energy scattering parameters for the ion-atom system. It is found that the scattering length for the A$^2\Sigma_u^+$ state, $a_u$ = 1325 a$_0$, is positive and has well-constrained bounds. For the X$^2\Sigma_g^+$ state, the scattering length, $a_g$ = 20465 a$_0$ has a large magnitude as it is sensitive to the restrained change of the potential, due to the presence of a vibrational state in the vicinity of the dissociation limit., Comment: 10 pages, 7 figures, 4 tables

Femtochemistry techniques have been instrumental in accessing the short time scales necessary to probe transient intermediates in chemical reactions. Here we take the contrasting approach of prolonging the lifetime of an intermediate by preparing reactant molecules in their lowest ro-vibronic quantum state at ultralow temperatures, thereby drastically reducing the number of exit channels accessible upon their mutual collision. Using ionization spectroscopy and velocity-map imaging of a trapped gas of potassium-rubidium molecules at a temperature of 500~nK, we directly observe reactants, intermediates, and products of the reaction $^{40}$K$^{87}$Rb + $^{40}$K$^{87}$Rb $\rightarrow$ K$_2$Rb$^*_2$ $\rightarrow$ K$_2$ + Rb$_2$. Beyond observation of a long-lived energy-rich intermediate complex, this technique opens the door to further studies of quantum-state resolved reaction dynamics in the ultracold regime., Comment: 4 figures in main, 4 figures in SM, 2 table in SM

Atom-ion interactions occur through the electric dipole which is induced by the ion on the neutral atom. In a Langevin collision, in which the atom and ion overcome the centrifugal barrier and reach a short internuclear distance, their internal electronic states deform due to their interaction and can eventually alter. Here we explore the outcome products and the energy released from a single Langevin collision between a single cold $^{88}$Sr$^{+}$ ion initialized in the metastable $4d^2D_{5/2,3/2}$ states, and a cold $^{87}$Rb atom in the $5s^2S_{1/2}$ ground state. We found that the long-lived $D_{5/2}$ and $D_{3/2}$ states quench after roughly three Langevin collisions, transforming the excitation energy into kinetic energy. We identify two types of collisional quenching. One is an Electronic Excitation-Exchange process, during which the ion relaxes to the $S$ state and the atom is excited to the $P$ state, followed by energy release of $\sim$ 3000 K$\cdot$k$_B$. The second is Spin-Orbit Change where the ion relaxes from the higher fine-structure $D_{5/2}$ level to the lower $D_{3/2}$ level releasing $\sim$ 400 K$\cdot$k$_B$ into kinetic motion. These processes are theoretically understood to occur through Landau-Zener avoided crossings between the different molecular potential curves. We also found that these relaxation rates are insensitive to the mutual spin orientation of the ion and atoms. This is explained by the strong inertial Coriolis coupling present in ultracold atom-ion collisions due to the high partial wave involved, which strongly mixes different angular momentum states. This inertial coupling explains the loss of the total electronic angular-momentum which is transferred to the external rotation of nuclei. Our results provide deeper understanding of ultracold atom-ion inelastic collisions and offer additional quantum control tools for the cold chemistry field.

We study polar alkali dimer scattering in a quasi-1D geometry for both reactive and non-reactive species. Elastic and reactive rates are computed as a function of the amplitude of a static electric field within a purely long-range model with suitable boundary conditions at shorter range. We describe the diatomic molecules as rigid rotors and results are compared to the fixed-dipole approximation. We show in particular that for molecules with a sufficiently strong induced dipole moment oriented perpendicular to the trap axis, the long-range repulsive interaction leads to the suppression of short-range processes. Such shielding effect occurs for both reactive and non-reactive molecules, preventing two-body reactions as well as losses due to "sticky processes" [Phys. Rev. A 85, 062712 (2012)] from occurring. The present results demonstrate the possibility to suppress loss rates in current ultracold molecule experiments using 1D confinement., Comment: 17 pages, 8 figures

The dipolar collision between ultracold polar molecules is an important topic both by its own right from the fundamental point of view and for the successful exploration of many-body physics with strong and long-range dipolar interactions. Here, we report the investigation of collisions between ultracold ground-state sodium-rubidium molecules in electric fields with induced electric dipole moments as large as 0.7$\;$D. We observe a step-wise enhancement of losses due to the coupling between different partial waves induced by the increasingly stronger anisotropic dipolar interactions. Varying the temperature of our sample, we find good agreement with theoretical loss rates assuming complex formation as the main loss process. Our results shed new light on the understanding of complex molecular collisions in the presence of strong dipolar interactions and also demonstrate the versatility of modifying molecular interactions with electric fields., Comment: 8 pages, 4 figures, PRX in press

Two-dimensional electronic spectroscopy (2DES) is one of the most powerful spectroscopic techniques, capable of attaining a nearly complete picture of a quantum system including its couplings, quantum coherence properties and its real-time dynamics. While successfully applied to a variety of condensed phase samples, high precision experiments on isolated quantum systems in the gas phase have been so far precluded by insufficient sensitivity. However, such experiments are essential for a precise understanding of fundamental mechanisms and to avoid misinterpretations, e.g. as for the nature of quantum coherences in energy trans-port. Here, we solve this issue by extending 2DES to isolated nanosystems in the gas phase prepared by helium nanodroplet isolation in a molecular beam-type experiment. This approach uniquely provides high flexibility in synthesizing tailored, quantum state-selected model systems of single and many-body properties. For demonstration, we deduce a precise and conclusive picture of the ultrafast coherent dynamics in isolated high-spin Rb2 molecules and present for the first time a dynamics study of the system-bath interaction between a single molecule (here Rb3) and a superfluid helium environment. The results demonstrate the unique capacity to elucidate prototypical interactions and dynamics in tailored quantum systems and bridges the gap to experiments in ultracold quantum science.

We report a detailed molecular spectroscopy study on the lowest excited electronic states of $^{23}\rm{Na}^{87}\rm{Rb}$ for producing ultracold $^{23}\rm{Na}^{87}\rm{Rb}$ molecules in the electronic, rovibrational and hyperfine ground state. Starting from weakly-bound Feshbach molecules, a series of vibrational levels of the $A^{1}\Sigma^{+}-b^{3}\Pi$ coupled excited states were investigated. After resolving, modeling and interpreting the hyperfine structure of several lines, we successfully identified a long-lived level resulting from the accidental hyperfine coupling between the $0^+$ and $0^-$ components of the $b^3\Pi$ state, satisfying all the requirements for the population transfer toward the lowest rovibrational level of the X$^1\Sigma^+$ state. Using two-photon spectroscopy, its binding energy was measured to be 4977.308(3) cm$^{-1}$, the most precise value to date. We calibrated all the transition strengths carefully and also demonstrated Raman transfer of Feshbach molecules to the absolute ground state.

In this article we address the general approach for calculating dynamical dipole polarizabilities of small quantum systems, based on a sum-over-states formula involving in principle the entire energy spectrum of the system. We complement this method by a few-parameter model involving a limited number of effective transitions, allowing for a compact and accurate representation of both the isotropic and anisotropic components of the polarizability. We apply the method to the series of ten heteronuclear molecules composed of two of ($^7$Li,$^{23}$Na,$^{39}$K,$^{87}$Rb,$^{133}$Cs) alkali-metal atoms. We rely on both up-to-date spectroscopically-determined potential energy curves for the lowest electronic states, and on our systematic studies of these systems performed during the last decade for higher excited states and for permanent and transition dipole moments. Such a compilation is timely for the continuously growing researches on ultracold polar molecules. Indeed the knowledge of the dynamic dipole polarizabilities is crucial to model the optical response of molecules when trapped in optical lattices, and to determine optimal lattice frequencies ensuring optimal transfer to the absolute ground state of initially weakly-bound molecules. When they exist, we determine the so-called "magic frequencies" where the ac-Stark shift and thus the viewed trap depth, is the same for both weakly-bound and ground-state molecules., Comment: Accepted in International Reviews of Physical Chemistry

We report the successful production of an ultracold sample of absolute ground-state $^{23}$Na$^{87}$Rb molecules. Starting from weakly-bound Feshbach molecules formed via magneto-association, the lowest rovibrational and hyperfine level of the electronic ground state is populated following a high efficiency and high resolution two-photon Raman process. The high purity absolute ground-state samples have up to 8000 molecules and densities of over $10^{11}$ cm$^{-3}$. By measuring the Stark shifts induced by external electric fields, we determined the permanent electric dipole moment of the absolute ground-state $^{23}$Na$^{87}$Rb and demonstrated the capability of inducing an effective dipole moment over one Debye. Bimolecular reaction between ground-state $^{23}$Na$^{87}$Rb molecules is endothermic, but we still observed a rather fast decay of the molecular sample. Our results pave the way toward investigation of ultracold molecular collisions in a fully controlled manner, and possibly to quantum gases of ultracold bosonic molecules with strong dipolar interactions., Comment: 5pages, 5 figures

We report a high-resolution spectroscopic investigation of the long-range states of the $^{23}$Na$^{87}$Rb molecule near its Na($3^2S_{1/2}$)+Rb($5^2P_{3/2}$) asymptote. This study was performed with weakly bound ultracold molecules produced via magneto-association with an inter-species Feshbach resonance. We observed several regular vibrational series, which are assigned to the 5 attractive long-range states correlated with this asymptote. The vibrational levels of two of these states have sharp but complex structures due to hyperfine and Zeeman interactions. For the other states, we observed significant linewidth broadenings due to strong predissociation caused by spin-orbit couplings with states correlated to the lower Na($3^2S_{1/2}$)+Rb($5^2P_{1/2}$) asymptote. The long-range $C_6$ van der Waals coefficients extracted from our spectrum are in good agreement with theoretical values., Comment: Phys.Rev. A in press

The direct photodissociation of trapped $^{85}$Rb$_2^+$ (rubidium) molecular ions by the cooling light for the $^{85}$Rb magneto-optical trap (MOT) is studied, both experimentally and theoretically. Vibrationally excited Rb$_{2}^{+}$ ions are created by photoionization of Rb$_{2}$ molecules formed photoassociatively in the Rb MOT and are trapped in a modified spherical Paul trap. The decay rate of the trapped Rb$_{2}^{+}$ ion signal in the presence of the MOT cooling light is measured and agreement with our calculated rates for molecular ion photodissociation is observed. The photodissociation mechanism due to the MOT light is expected to be active and therefore universal for all homonuclear diatomic alkali metal molecular ions.

A model for determining the hyperfine structure of the excited electronic states of diatomic bialkali heteronuclear molecules is formulated from the atomic hyperfine interactions, and is applied to the case of bosonic $^{39}$KCs and fermionic $^{40}$KCs molecules. The hyperfine structure of the potential energy curves of the states correlated to the K($4s\,^2S_{1/2}$)+Cs($6p\,^2P_{1/2,3/2}$) dissociation limits is described in terms of different coupling schemes depending on the internuclear distance $R$. These results provide the first step in the calculation of the hyperfine structure of rovibrational levels of these excited molecular states in the perspective of the identification of efficient paths for creating ultracold ground-state KCs molecules., Comment: 12 pages, 15 figures

We have calculated the isotropic $C\_6$ 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 $X^1\Sigma^+$. We consider the ten species made up of $^7$Li, $^{23}$Na, $^{39}$K, $^{87}$Rb and $^{133}$Cs. Following our previous work [M.~Lepers \textit{et.~al.}, Phys.~Rev.~A \textbf{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.

Heteronuclear alkali-metal dimers represent the class of molecules of choice for creating samples of ultracold molecules exhibiting an intrinsic large permanent electric dipole moment. Among them, the KCs molecule, with a permanent dipole moment of 1.92~Debye still remains to be observed in ultracold conditions. Based on spectroscopic studies available in the literature completed by accurate quantum chemistry calculations, we propose several optical coherent schemes to create ultracold bosonic and fermionic KCs molecules in their absolute rovibrational ground level, starting from a weakly bound level of their electronic ground state manifold. The processes rely on the existence of convenient electronically excited states allowing an efficient stimulated Raman adiabatic transfer of the level population.

We study, both theoretically and experimentally, the dynamical polarizability $\alpha(\omega)$ of $\textrm{Rb}_2$ molecules in the rovibrational ground state of $\mathrm{a}^3\Sigma_u^+$. Taking all relevant excited molecular bound states into account, we compute the complex-valued polarizability $\alpha(\omega)$ for wave numbers up to $20000\:\textrm{cm}^{-1}$. Our calculations are compared to experimental results at $1064.5\:\textrm{nm}$ ($\sim9400\:\textrm{cm}^{-1}$) as well as at $830.4\:\textrm{nm}$ ($\sim12000\:\textrm{cm}^{-1}$). Here, we discuss the measurements at $1064.5\:\textrm{nm}$. The ultracold $\textrm{Rb}_2$ molecules are trapped in the lowest Bloch band of a 3D optical lattice. Their polarizability is determined by lattice modulation spectroscopy which measures the potential depth for a given light intensity. Moreover, we investigate the decay of molecules in the optical lattice, where lifetimes of more than $2\:\textrm{s}$ are observed. In addition, the dynamical polarizability for the $\mathrm{X}^1\Sigma_g^+$ state is calculated. We provide simple analytical expressions that reproduce the numerical results for $\alpha(\omega)$ for all vibrational levels of $\mathrm{a}^3\Sigma_u^+$ as well as $\mathrm{X}^1\Sigma_g^+$. Precise knowledge of the molecular polarizability is essential for designing experiments with ultracold molecules as lifetimes and lattice depths are key parameters. Specifically the wavelength at $\sim1064\:\textrm{nm}$ is of interest, since here, ultrastable high power lasers are available., Comment: 22 pages, 10 figures

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. 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., Comment: 9 pages, 5 figures

We perform one- and two-photon high resolution spectroscopy on ultracold samples of RbCs Feshbach molecules with the aim to identify a suitable route for efficient ground-state transfer in the quantum-gas regime to produce quantum gases of dipolar RbCs ground-state molecules. One-photon loss spectroscopy allows us to probe deeply bound rovibrational levels of the mixed excited (A1{\Sigma}+ - b3{\Pi}0) 0+ molecular states. Two-photon dark state spectroscopy connects the initial Feshbach state to the rovibronic ground state. We determine the binding energy of the lowest rovibrational level |v"=0,J"=0> of the X1{\Sigma}+ ground state to be DX 0 = 3811.5755(16) 1/cm, a 300-fold improvement in accuracy with respect to previous data. We are now in the position to perform stimulated two-photon Raman transfer to the rovibronic ground state., Comment: Submitted to PCCP themed issue: Physics and Chemistry of Cold Molecules

The present paper aims at finding optimal parameters for trapping of Cs$_2$ molecules in optical lattices, with the perspective of creating a quantum degenerate gas of ground-state molecules. We have calculated dynamic polarizabilities of Cs$_2$ molecules subject to an oscillating electric field, using accurate potential curves and electronic transition dipole moments. We show that for some particular wavelengths of the optical lattice, called "magic wavelengths", the polarizability of the ground-state molecules is equal to the one of a Feshbach molecule. As the creation of the sample of ground-state molecules relies on an adiabatic population transfer from weakly-bound molecules created on a Feshbach resonance, such a coincidence ensures that both the initial and final states are favorably trapped by the lattice light, allowing optimized transfer in agreement with the experimental observation.

The electrostatic interaction between an excited atom and a diatomic ground state molecule in an arbitrary rovibrational level at large mutual separations is investigated with a general second-order perturbation theory, in the perspective of modeling the photoassociation between cold atoms and molecules. We find that the combination of quadrupole-quadrupole and van der Waals interactions compete with the rotational energy of the dimer, limiting the range of validity of the perturbative approach to distances larger than 100 a.u.. Numerical results are given for the long-range interaction between Cs and Cs$_2$, showing that the photoassociation is probably efficient whatever the Cs$_2$ rotational energy., Comment: 6 figures, 2 tables