arXiv subjects

Goulven Quéméner

Publications and source records attributed to Goulven Quéméner.

At least 37 records · Page 2Linked to original sources

arXiv2018

Collisions of ultracold ^{23}Na^{87}Rb molecules with controlled chemical reactivities

The collision of molecules at ultracold temperatures is of great importance for understanding the chemical interactions at the quantum regime. While much theoretical work has been devoted to this, experimental data are only available sparsely mainly due to the difficulty in producing ground-state molecules at ultracold temperatures. We report here the creation of optically trapped samples of ground-state bosonic sodium-rubidium molecules with precisely controlled internal states and, enabled by this, a detailed study on the inelastic loss with and without the NaRb + NaRb $\rightarrow$ Na$_2$ + Rb$_2$ chemical reaction. Contrary to intuitive expectations, we observed very similar loss and heating, regardless of the chemical reactivities. In addition, as evidenced by the reducing loss rate constants with increasing temperatures, we found that these collisions are already outside the Wigner region even though the sample temperatures are sub-microkelvin. Our measurement agrees semi-quantitatively with models based on long-range interactions, but calls for a deeper understanding on the short-range physics for a more complete interpretation.

cond-mat.quant-gas↗

arXiv2017

High-resolution Internal State Control of Ultracold $^{23}$Na$^{87}$Rb Molecules

We report the full control over the internal states of ultracold $^{23}$Na$^{87}$Rb molecules, including vibrational, rotational and hyperfine degrees of freedom. Starting from a sample of weakly bound Feshbach molecules, we realize the creation of molecules in single hyperfine levels of both the rovibrational ground and excited states with a high-efficiency and high-resolution stimulated Raman adiabatic passage. Starting from the rovibrational and hyperfine ground state, we demonstrate rotational and hyperfine control with one- and two-photon microwave spectroscopy. This achievement of fully controlling the molecular internal states paves the way to study state dependent molecular collisions and state controlled chemical reactions.

cond-mat.quant-gas↗

arXiv2017

Adimensional theory of shielding in ultracold collisions of dipolar rotors

We investigate the electric field shielding of ultracold collisions of dipolar rotors, initially in their first rotational excited state, using an adimensional approach. We establish a map of good and bad candidates for efficient evaporative cooling based on this shielding mechanism, by presenting the ratio of elastic over quenching processes as a function of a rescaled rotational constant $\tilde{B} = B/s_{E_3}$ and a rescaled electric field $\tilde{F} = dF/B$. $B, d, F, s_{E_3}$ are respectively the rotational constant, the full electric dipole moment of the molecules, the applied electric field and a characteristic dipole-dipole energy. We identify two groups of bi-alkali dipolar molecules. The first group, including RbCs, NaK, KCs, LiK, NaRb, LiRb, NaCs and LiCs, is favorable with a ratio over 1000 at collision energies equal (or even higher) to their characteristic dipolar energy. The second group, including LiNa and KRb, is not favorable. More generally, for molecules well described by Hund's case b, our adimensional study provides the conditions of efficient evaporative cooling. The range of appropriate rescaled rotational constant and rescaled field is approximately $\tilde{B} \ge 10^8$ and $3.25 \le \tilde{F} \le 3.8$, with a maximum ratio reached for $\tilde{F} \simeq 3.4$ for a given $\tilde{B}$. We also discuss the importance of the electronic van der Waals interaction on the adimensional character of our study.

physics.atom-ph↗

arXiv2017

Ultracold collisions of molecules

This paper deals with the theory of collisions between two ultracold particles with a special focus on molecules. It describes the general features of the scattering theory of two particles with internal structure, using a time-independent quantum formalism. It starts from the Schrödinger equation and introduces the experimental observables such as the differential or integral cross sections, and rate coefficients. Using a partial-wave expansion of the scattering wavefunction, the radial motion of the collision is described through a linear system of coupled equations, which is solved numerically. Using a matching procedure of the scattering wavefunction with its asymptotic form, the observables such as cross sections and rate coefficients are obtained from the extraction of the reactance, scattering and transition matrices. The example of the collision of two dipolar molecules in the presence of an electric field is presented, showing how dipolar interactions and collisions can be controlled.

physics.atom-ph↗

arXiv2016

Creation of an ultracold gas of ground-state $^{23}\rm{Na}^{87}\rm{Rb}$ molecules

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.

cond-mat.quant-gas↗

arXiv2015

Shielding $^2Σ$ ultracold dipolar molecular collisions with electric fields

The prospects for shielding ultracold, paramagnetic, dipolar molecules from inelastic and chemical collisions are investigated. Molecules placed in their first rotationally excited states are found to exhibit effective long-range repulsion for applied electric fields above a certain critical value, as previously shown for non-paramagnetic molecules. This repulsion can safely allow the molecules to scatter while reducing the risk of inelastic or chemically reactive collisions. Several molecular species of $^2Σ$ molecules of experimental interest -- RbSr, SrF, BaF, and YO -- are considered, and all are shown to exhibit orders of magnitude suppression in quenching rates in a sufficiently strong laboratory electric field. It is further shown that, for these molecules described by Hund's coupling case b, electronic and nuclear spins play the role of spectator with respect to the shielding.

physics.atom-ph↗

arXiv2015

Four-body long-range interactions between ultracold weakly-bound diatomic molecules

Using the multipolar expansion of electrostatic and magnetostatic potential energies, we characterize the long-range interactions between two weakly-bound diatomic molecules, taking as an example the paramagnetic Er$_2$ Feshbach molecules which were produced recently. Since inside each molecule, individual atoms conserve their identity, the intermolecular potential energy can be expanded as the sum of pairwise atomic potential energies. In the case of Er$_2$ Feshbach molecules, we show that the interaction between atomic magnetic dipoles gives rise to the usual $R^{-3}$ term of the multipolar expansion, with $R$ the intermolecular distance, but also to additional terms scaling as $R^{-5}$, $R^{-7}$, and so on. Those terms are due to the interaction between effective molecular multipole moments, and are strongly anisotropic with respect to the orientation of the molecules. Similarly the atomic pairwise van der Waals interaction results in $R^{-6}$, $R^{-8}$, ... terms in the intermolecular potential energy. By calculating the reduced electric-quadrupole moment of erbium ground level $\langle J=6||\hat{Q}_2||J=6\rangle = -1.305$ a.u., we also demonstrate that the electric-quadrupole interaction energy is negligible with respect to the magnetic-dipole and van der Waals interaction energies. The general formalism presented in this article can be applied to calculate the long-range potential energy between arbitrary charge distributions composed of almost free subsystems.

physics.atom-ph↗

arXiv2015

Dynamics of ultracold dipolar particles in a confined geometry and tilted fields

We develop a collisional formalism adapted for the dynamics of ultracold dipolar particles in a confined geometry and in fields tilted relative to the confinement axis. Using tesseral harmonics instead of the usual spherical harmonics to expand the scattering wavefunction, we recover a good quantum number $ξ= \pm 1$ which is conserved during the collision. We derive the general expression of the dipole-dipole interaction in this convenient basis set as a function of the polar and azimuthal angles of the fields. We apply the formalism to the collision of fermionic and bosonic polar KRb molecules in a tilted electric field and in a one-dimensional optical lattice. The presence of a tilted field drastically changes the magnitude of the reactive and inelastic rates as well as the inelastic threshold properties at vanishing collision energies. Setting an appropriate strength of the confinement for the fermionic system, we show that the ultracold particles can even further reduce their kinetic energy by inelastic excitation to higher states of the confinement trap.

physics.atom-ph↗

arXiv2014

Tuning ultracold collisions of excited rotational dipolar molecules

We investigate the ultracold collisions of rotationally excited dipolar molecules in free-space, taking the hetero-nuclear bi-alkali molecule of KRb as an example. We show that we can sharply tune the elastic, inelastic and reactive rate coefficients of lossy molecular collisions when a second rotationally excited colliding channel crosses the threshold of the initial colliding channel, with the help of an applied electric field, as found by Avdeenkov et al. for non-lossy molecules [Phys. Rev. A 73, 022707 (2006)]. We can increase or decrease the loss processes whether the second channel is above or below the initial channel. This is seen for both bosonic and fermionic molecules. Additionally, we include the electric quadrupole and octopole moment to the dipole moment in the expression of the long-range multipole-multipole interaction. We found that for processes mediated by the incident channel like elastic and loss collisions, the inclusion of quadrupole and octopole moments are not important at ultralow energies. They are important for processes mediated by state-to-state transitions like inelastic collisions.

physics.atom-ph↗

arXiv2013

Evaporative cooling of reactive polar molecules confined in a two-dimensional geometry

Recent experimental developments in the loading of ultracold KRb molecules into quasi-two-dimensional traps, combined with the ability to tune the ratio between elastic and loss (inelastic/reactive) collisions through application of an external electric field, are opening the door to achieving efficient evaporative cooling of reactive polar molecules. In this paper, we use Monte Carlo simulations and semianalytic models to study theoretically the experimental parameter regimes in which evaporative cooling is feasible under current trapping conditions. We investigate the effect of the anisotropic character of dipole-dipole collisions and reduced dimensionality on evaporative cooling. We also present an analysis of the experimentally relevant anti-evaporation effects that are induced by chemical reactions that take place when more than one axial vibrational state is populated.

quant-ph↗

arXiv2013

Ultracold molecular collisions in combined electric and magnetic fields

We consider collisions of electric and magnetic polar molecules, taking the OH radical as an example, subject to combined electric and magnetic static fields. We show that the relative orientation of the fields has an important effect on the collision processes for different fields magnitude at different collision energies. This is due to the way the molecules polarize in the combined electric and magnetic fields and hence the way the electric dipole-dipole interaction rises. If OH molecules are confined in magnetic quadrupole traps and if an electric field is applied, molecular collisions will strongly depend on the position as well as the velocity of the molecules, and consequences on the molecular dynamics are discussed.

physics.atom-ph↗

arXiv2013

Dipolar Radicals in Crossed Electric and Magnetic Fields

Paramagnetic, dipolar Hund's case-a radicals are considered in the presence of arbitrary, non-collinear combinations of electric and magnetic fields. The field-dependent part of the Hamiltonian is found to be exactly diagonalizable, and described by quantum numbers given by the projection of the molecule's total angular momentum along a space-fixed axis that is determined by both the fields and the electric and magnetic dipole moments of the molecule. In cases of strong fields, this procedure identifies a set of quantum numbers for the molecule in crossed fields. We dub this set a "Hund's case-X" basis.

quant-ph↗

arXiv2012

Überresonant Scattering of Ultracold Molecules

Compared to purely atomic collisions, ultracold molecular collisions potentially support a much larger number of Fano-Feshbach resonances due to the enormous number of ro-vibrational states available. In fact, for alkali-metal dimers we find that the resulting density of resonances cannot be resolved at all, even on the sub-$μ$K temperature scale of ultracold experiments. As a result, all observables become averaged over many resonances and can effectively be described by simpler, non-resonant scattering calculations. Two particular examples are discussed: non-chemically reactive RbCs and chemically reactive KRb. In the former case, the formation of a long-lived collision complex may lead to the ejection of molecules from a trap. In the latter case, chemical reactions broaden the resonances so much that they become unobservable.

physics.atom-ph↗

arXiv2012

Evaporative cooling of the dipolar radical OH

Atomic physics was revolutionized by the development of forced evaporative cooling: it led directly to the observation of Bose-Einstein condensation, quantum-degenerate Fermi gases, and ultracold optical lattice simulations of condensed matter phenomena. More recently, great progress has been made in the production of cold molecular gases, whose permanent electric dipole moment is expected to generate rich, novel, and controllable phases, dynamics, and chemistry in these ultracold systems. However, while many strides have been made in both direct cooling and cold-association techniques, evaporative cooling has not yet been achieved due to unfavorable elastic-to-inelastic ratios and impractically slow thermalization rates in the available trapped species. We now report the observation of microwave-forced evaporative cooling of hydroxyl (OH) molecules loaded from a Stark-decelerated beam into an extremely high-gradient magnetic quadrupole trap. We demonstrate cooling by at least an order of magnitude in temperature and three orders in phase-space density, limited only by the low-temperature sensitivity of our spectroscopic thermometry technique. With evaporative cooling and sufficiently large initial populations, much colder temperatures are possible, and even a quantum-degenerate gas of this dipolar radical -- or anything else it can sympathetically cool -- may now be in reach.

physics.atom-ph↗

arXiv2011

Universalities in ultracold reactions of alkali polar molecules

We consider ultracold collisions of ground-state, heteronuclear alkali dimers that are susceptible to four-center chemical reactions 2 AB -> A2 + B2 even at sub-microKelvin temperature. These reactions depend strongly on species, temperature, electric field, and confinement in an optical lattice. We calculate ab initio van der Walls coefficients for these interactions, and use a quantum formalism to study the scattering properties of such molecules under an external electric field and optical lattice. We also apply a quantum threshold model to explore the dependence of reaction rates on the various parameters. We find that, among the heteronuclear alkali fermionic species, LiNa is the least reactive, whereas LiCs is the most reactive. For the bosonic species, LiK is the most reactive in zero field, but all species considered - LiNa, LiK, LiRb, LiCs, and KRb - share a universal reaction rate once a sufficiently high electric field is applied.

physics.atom-ph↗

arXiv2011

Inelastic collisions and density-dependent excitation suppression in a ${}^{87}$Sr optical lattice clock

We observe two-body loss of ${}^3P_0$ ${}^{87}$Sr atoms trapped in a one-dimensional optical lattice. We measure loss rate coefficients for atomic samples between 1 and 6 $μ$K that are prepared either in a single nuclear-spin-sublevel or with equal populations in two sublevels. The measured temperature and nuclear spin preparation dependence of rate coefficients agree well with calculations and reveal that rate coefficients for distinguishable atoms are only slightly enhanced over those of indistinguishable atoms. We further observe a suppression of excitation and losses during interrogation of the ${}^1S_0$-${}^3P_0$ transition as density increases and Rabi frequency decreases, which suggests the presence of strong interactions in our dynamically driven many-body system.

physics.atom-ph↗

arXiv2010

Dynamics of ultracold molecules in confined geometry and electric field

We present a time-independent quantum formalism to describe the dynamics of molecules with permanent electric dipole moments in a two-dimensional confined geometry such as a one-dimensional optical lattice, in the presence of an electric field. Bose/Fermi statistics and selection rules play a crucial role in the dynamics. As examples, we compare the dynamics of confined fermionic and bosonic polar KRb molecules under different confinements and electric fields. We show how chemical reactions can be suppressed, either by a "statistical suppression" which applies for fermions at small electric fields and confinements, or by a "potential energy suppression", which applies for both fermions and bosons at high electric fields and confinements. We also explore collisions that transfer molecules from one state of the confining potential to another. Although these collisions can be significant, we show that they do not play a role in the loss of the total number of molecules in the gas.

physics.atom-ph↗

arXiv2010

A Simple Quantum Model of Ultracold Polar Molecule Collisions

We present a unified formalism for describing chemical reaction rates of trapped, ultracold molecules. This formalism reduces the scattering to its essential features, namely, a propagation of the reactant molecules through a gauntlet of long-range forces before they ultimately encounter one another, followed by a probability for the reaction to occur once they do. In this way, the electric-field dependence should be readily parametrized in terms of a pair of fitting parameters (along with a $C_6$ coefficient) for each asymptotic value of partial wave quantum numbers $|L,M \rangle$. From this, the electric field dependence of the collision rates follows automatically. We present examples for reactive species such as KRb, and non-reactive species, such as RbCs.

quant-ph↗