The authors show that a precise microwave preparation of a quantum superposition between three rotational states of an ultracold dipolar molecule generates controllable interferences in their calculated collisional rate coefficients, at an electric field that produces a F\"orster resonance. This can enable coherent control on ultracold molecular collisions in current experiments.
The authors show that a precise microwave preparation of a quantum superposition between three rotational states of an ultracold dipolar molecule generates controllable interferences in their calculated collisional rate coefficients, at an electric field that produces a F"orster resonance. This can enable coherent control on ultracold molecular collisions in current experiments.
We propose a one-channel, simple model to describe the dynamics of ultracold dipolar molecules around a F\"orster resonance. Slightly above a specific electric field, a collisional shielding can take place, suppressing the molecular losses in a gas. The overall description of the quantum physical mechanism comes back to the dynamics on a unique energy surface, which depends on the relative distance and angular approach of the molecules. This surface enables us to interpret how the dipole moments of the molecules are induced and interlocked by the electric field and the dipole-dipole interaction during the process, especially when the shielding is triggered. Averaging the relative angular motion over a unique partial wave (the lowest one when the ultracold regime is reached), the model reproduces well the behavior of the rate coefficients observed experimentally and predicted theoretically [K. Matsuda, L. De Marco, J.-R. Li, W. G. Tobias, G. Valtolina, G. Qu\'em\'ener, and J. Ye, Science 370, 1324 (2020); J.-R. Li, W. G. Tobias, K. Matsuda, C. Miller, G. Valtolina, L. D. Marco, R. R. W. Wang, L. Lassabli\`ere, G. Qu\'em\'ener, J. L. Bohn, and J. Ye, Nat. Phys. 17, 1144 (2021)]. This economic model encapsulates the main physics of the quantum process. Therefore, it can be used as an alternative to a full quantum dynamical treatment and is promising for future studies of collisions involving more bodies.
We propose a method to suppress collisional loss in strongly dipolar, rotationally excited ultracold molecules using a combination of static (dc) and microwave (ac) electric fields. By tuning two excited pair molecular rotational states into a Förster resonance with a dc field, simultaneously driving excited rotational transitions with an ac field removes all long-range bound states, allowing near complete suppression of all two- and three-body collisional loss channels. While permitting tunable dipolar and anti-dipolar interactions, this bound-state-free ac/dc scheme is not subject to photon-changing collisions that are the primary source of two-body loss in shielding with two microwave fields, used to achieve the first molecular Bose-Einstein condensate [Bigagli et al., Nature 631, 289 (2024)]. Using NaCs as a representative example for strongly dipolar molecules, close-coupling calculations are performed to show that bound-state-free shielding can achieve ratios of elastic-to-loss rates ≳106 at 100 nK, with currently accessible ac and dc field generation technologies. This work opens new opportunities for realizing large, long-lived samples of strongly interacting degenerate molecular gases with tunable long-range interactions.
This thesis presents the development of a toolbox for the coherent control of ultracold polar molecules. Such systems of molecules promise the creation of long-lived, highly dipolar quantum gases with applications spanning the fields of quantum state controlled chemistry, quantum information, quantum simulation, and precision measurement. However, the addition of vibrational and rotational degrees of freedom leads to molecular systems being significantly more complex than their widely used atomic counterparts. In this work we demonstrate full control of the quantum state down to the hyperfine level of an optically trapped sample of ultracold bosonic 87Rb133 Cs molecules, and exploit that control to begin an investigation into the collision processes which take place in an ultracold molecular gas. We create a sample of up to ∼ 4000 optically trapped molecules in their rovibronic and hyperfine ground state. We characterise the molecules by measuring their temperature, binding energy, and molecule-frame electric dipole moment. We perform spectroscopy of the first rotationally excited state with hyperfine state resolution using microwaves to determine accurate values of rotational and hyperfine coupling constants. We use coherent π pulses to perform complete transfer population between selected hyperfine levels of the ground, first-excited, and second-excited rotational states. We investigate the effect of the off-resonant light of our optical dipole trap on the rotational and hyperfine structure of the molecules. Through a combination of high-resolution microwave spectroscopy and parametric heating measurements, we characterise the polarisability of the 87Rb133Cs molecule. We demonstrate that coupling between neighbouring hyperfine states manifests in rich structure with many avoided crossings in any rotational state other than the ground state. This coupling may be tuned by rotating the polarisation of the linearly polarised trapping light. Finally, we study the lifetime of polar bosonic 87Rb133Cs molecules in our 3D optical dipole trap. We examine the lifetime of the molecules as a function of dipole trap intensity, magnetic field, and hyperfine and rotational state. Despite the chemical stability of the 87Rb133 Cs molecule, we observe lifetimes of ∼1 s corresponding to 2-body decay rates close to the universal limit.
Full control of molecular interactions, including reactive losses, would open new frontiers in quantum science. We demonstrate extreme tunability of ultracold chemical reaction rates by inducing resonant dipolar interactions by means of an external electric field. We prepared fermionic potassium-rubidium molecules in their first excited rotational state and observed a modulation of the chemical reaction rate by three orders of magnitude as we tuned the electric field strength by a few percent across resonance. In a quasi-two-dimensional geometry, we accurately determined the contributions from the three dominant angular momentum projections of the collisions. Using the resonant features, we shielded the molecules from loss and suppressed the reaction rate by an order of magnitude below the background value, thereby realizing a long-lived sample of polar molecules in large electric fields.
We demonstrate microwave dressing on ultracold, fermionic ^{23}Na^{40}K ground-state molecules and observe resonant dipolar collisions with cross sections exceeding 3 times the s-wave unitarity limit. The origin of these interactions is the resonant alignment of the approaching molecules' dipoles along the intermolecular axis, which leads to strong attraction. We explain our observations with a conceptually simple two-state picture based on the Condon approximation. Furthermore, we perform coupled-channel calculations that agree well with the experimentally observed collision rates. The resonant microwave-induced collisions found here enable controlled, strong interactions between molecules, of immediate use for experiments in optical lattices.
Ultracold polar molecular gases promise new directions and exciting appli-cations in precision measurements, ultracold chemistry, electric-field controlled collisions, dipolar quantum gases, and quantum information sciences. This the-sis presents experimental realization of a near quantum degenerate gas of polar molecules, where the phase-space density of the gas achieved is more than 10 or-ders of magnitude higher than previous results. The near quantum degenerate gas of polar molecules is created using two coherent steps. First, atoms in an ul-tracold gas mixture are converted into extremely weakly bound molecules near a Fano-Feshbach resonance. Second, the weakly bound molecules are transferred to the ro-vibronic ground state using a coherent two-photon Raman technique. The fact that these ground-state molecules are polar is confirmed with a spectroscopic measurement of the permanent electric dipole moment. Finally, manipulation of the molecular hyperfine state is demonstrated; this allows molecules to be pop-ulated in a single quantum state, in particular, the lowest energy state. With an ultracold gas of molecules, full control of molecular internal state, and electric field as a new handle, ultracold molecular collisions, including ultracold chemical reactions and dipolar collisions, are studied.