Goulven Quéméner

Quantum-State Controlled Chemical Reactions of Ultracold Potassium-Rubidium Molecules

Colliding in the Cold Chemical reactions occur through molecular collisions, which, in turn, are governed by the distributions of energy in each colliding partner. What happens when molecules are cooled so that they no longer have sufficient energy to collide? Ospelkaus et al. (p. 853; see the Perspective by Hutson) explored this question by preparing a laser-cooled sample of potassium rubidium (KRb) diatomics with barely any residual energy in any form (translational, rotational, vibrational, or electronic). By monitoring heat release over time, evidence was gathered for exothermic atom exchange reactivity through quantum mechanical tunneling. As predicted by theory, these reactions were exquisitely sensitive to the molecular states, with rates changing by orders of magnitude on varying minor factors such as nuclear spin orientation. Reactions mediated by quantum mechanical tunneling are observed, even in a sample of molecules cooled almost to a standstill. How does a chemical reaction proceed at ultralow temperatures? Can simple quantum mechanical rules such as quantum statistics, single partial-wave scattering, and quantum threshold laws provide a clear understanding of the molecular reactivity under a vanishing collision energy? Starting with an optically trapped near–quantum-degenerate gas of polar 40K87Rb molecules prepared in their absolute ground state, we report experimental evidence for exothermic atom-exchange chemical reactions. When these fermionic molecules were prepared in a single quantum state at a temperature of a few hundred nanokelvin, we observed p-wave–dominated quantum threshold collisions arising from tunneling through an angular momentum barrier followed by a short-range chemical reaction with a probability near unity. When these molecules were prepared in two different internal states or when molecules and atoms were brought together, the reaction rates were enhanced by a factor of 10 to 100 as a result of s-wave scattering, which does not have a centrifugal barrier. The measured rates agree with predicted universal loss rates related to the two-body van der Waals length.

Dipolar collisions of polar molecules in the quantum regime

Ultracold polar molecules offer the possibility of exploring quantum gases with interparticle interactions that are strong, long-range and spatially anisotropic. This is in stark contrast to the much studied dilute gases of ultracold atoms, which have isotropic and extremely short-range (or ‘contact’) interactions. Furthermore, the large electric dipole moment of polar molecules can be tuned using an external electric field; this has a range of applications such as the control of ultracold chemical reactions, the design of a platform for quantum information processing and the realization of novel quantum many-body systems. Despite intense experimental efforts aimed at observing the influence of dipoles on ultracold molecules, only recently have sufficiently high densities been achieved. Here we report the experimental observation of dipolar collisions in an ultracold molecular gas prepared close to quantum degeneracy. For modest values of an applied electric field, we observe a pronounced increase in the loss rate of fermionic potassium–rubidium molecules due to ultracold chemical reactions. We find that the loss rate has a steep power-law dependence on the induced electric dipole moment, and we show that this dependence can be understood in a relatively simple model based on quantum threshold laws for the scattering of fermionic polar molecules. In addition, we directly observe the spatial anisotropy of the dipolar interaction through measurements of the thermodynamics of the dipolar gas. These results demonstrate how the long-range dipolar interaction can be used for electric-field control of chemical reaction rates in an ultracold gas of polar molecules. Furthermore, the large loss rates in an applied electric field suggest that creating a long-lived ensemble of ultracold polar molecules may require confinement in a two-dimensional trap geometry to suppress the influence of the attractive, ‘head-to-tail’, dipolar interactions.

Ultracold Molecules under Control

1. Unconventional Conditions at Ultracold Temperatures 4949 1.

Controlling the Hyperfine State of Rovibronic Ground-State Polar Molecules

We report the preparation of a rovibronic ground-state molecular quantum gas in a single hyperfine state and, in particular, the absolute lowest quantum state. This addresses the last internal degree of freedom remaining after the recent production of a near quantum degenerate gas of molecules in their rovibronic ground state, and provides a crucial step towards full control over molecular quantum gases. We demonstrate a scheme that is general for bialkali polar molecules and allows the preparation of molecules in a single hyperfine state or in an arbitrary coherent superposition of hyperfine states. The scheme relies on electric-dipole, two-photon microwave transitions through rotationally excited states and makes use of electric nuclear quadrupole interactions to transfer molecular population between different hyperfine states.

Evaporative cooling of the dipolar hydroxyl radical

Atomic physics was revolutionized by the development of forced evaporative cooling, which led directly to the observation of Bose–Einstein condensation, quantum-degenerate Fermi gases and ultracold optical lattice simulations of condensed-matter phenomena. More recently, substantial progress has been made in the production of cold molecular gases. Their permanent electric dipole moment is expected to generate systems with varied and controllable phases, dynamics and chemistry. However, although advances have been made in both direct cooling and cold-association techniques, evaporative cooling has not been achieved so far. This is due to unfavourable ratios of elastic to inelastic scattering and impractically slow thermalization rates in the available trapped species. Here we report the observation of microwave-forced evaporative cooling of neutral hydroxyl (OH•) molecules loaded from a Stark-decelerated beam into an extremely high-gradient magnetic quadrupole trap. We demonstrate cooling by at least one order of magnitude in temperature, and a corresponding increase in phase-space density by three orders of magnitude, limited only by the low-temperature sensitivity of our spectroscopic thermometry technique. With evaporative cooling and a sufficiently large initial population, much colder temperatures are possible; even a quantum-degenerate gas of this dipolar radical (or anything else it can sympathetically cool) may be within reach.

Ultracold quantum dynamics: spin-polarized K + K_2 collisions with three identical bosons or fermions

We have developed a new potential energy surface for spin-polarized K(

Strong dependence of ultracold chemical rates on electric dipole moments

^2

Simple quantum model of ultracold polar molecule collisions

S) + K

Ultracold Dipolar Molecules Composed of Strongly Magnetic Atoms.

_{2}(^3\Sigma^+_u)

Quantum calculations of H2–H2 collisions: From ultracold to thermal energies

collisions and carried out quantum dynamical calculations of vibrational quenching at low and ultralow collision energies for both bosons