Sympathetic Cooling and Slowing of Molecules with Rydberg Atoms.

We propose to sympathetically slow and cool polar molecules in a cold, low-density beam using laser-cooled Rydberg atoms. The elastic collision cross sections between molecules and Rydberg atoms are large enough to efficiently thermalize the molecules even in a low-density environment. Molecules traveling at 100 m/s can be stopped in under 30 collisions with little inelastic loss. Our method does not require photon scattering from the molecules and can be generically applied to complex species for applications in precision measurement, quantum information science, and controlled chemistry.

Effective Three-Body Interactions in Cs(6s)-Cs(nd) Rydberg Trimers.

Ultralong-range Rydberg trimer molecules are spectroscopically observed in an ultracold gas of Cs(nd_{3/2}) atoms. The anisotropy of the atomic Rydberg state allows for the formation of angular trimers, whose energies may not be obtained from integer multiples of dimer energies. These nonadditive trimers coexist with Rydberg dimers. The existence of such effective three-body interactions is confirmed with the observation of asymmetric line profiles and interpreted by a theoretical approach that includes relativistic spin interactions. Simulations of the observed spectra with and without angular trimer lines lend convincing support to the existence of effective three-body interactions.

Theory of Ultralong-Range Rydberg Molecule Formation Incorporating Spin-Dependent Relativistic Effects: Cs(6s)-Cs(np) as Case Study.

We calculate vibrational spectra of ultralong-range Cs(32p) Rydberg molecules that form in an ultracold gas of Cs atoms. We account for the partial-wave scattering of the Rydberg electrons from the Cs perturber atoms by including the full set of spin-resolved 1,3 SJ and 1,3 PJ scattering phase shifts, and allow for the mixing of singlet (S=0) and triplet (S=1) spin states through Rydberg electron spin-orbit and ground state electron hyperfine interactions. Excellent agreement with observed data in Saßmannshausen et al. [Phys. Rev. Lett. 2015, 113, 133201] in line positions and profiles is obtained. We also determine the spin-dependent permanent electric dipole moments for these molecules. This is the first such calculation of ultralong-range Rydberg molecules for which all of the relativistic contributions are accounted.

Spin waves and dielectric softening of polar molecule condensates.

We consider an oblate Bose-Einstein condensate of heteronuclear polar molecules in a weak applied electric field. This system supports a rich quasiparticle spectrum that plays a critical role in determining its bulk dielectric properties. In particular, in sufficiently weak fields the system undergoes a polarization wave rotonization, leading to the development of textured electronic structure and a dielectric instability that is characteristic of the onset of a negative static dielectric function.

First-order phase transitions in optical lattices with tunable three-body onsite interaction.

We study the two-dimensional Bose-Hubbard model in the presence of a three-body interaction term, both at a mean-field level and via quantum Monte Carlo simulations. The three-body term is tuned by coupling the triply occupied states to a trapped universal trimer. We find that, for a sufficiently attractive three-body interaction, the n=2 Mott lobe disappears and the system displays first-order phase transitions separating the n=1 from the n=3 lobes and the n=1 and n=3 Mott insulator from the superfluid. We also analyze the effect of finite temperature and find that transitions are still of first order at temperatures T~J, where J is the hopping matrix element.

Rydberg atom mediated polar molecule interactions: a tool for molecular-state conditional quantum gates and individual addressability.

We study the possibility to use interaction between a polar molecule in the ground electronic and vibrational state and a Rydberg atom to construct two-qubit gates between molecular qubits and to coherently control molecular states. A polar molecule within the electron orbit in a Rydberg atom can either shift the Rydberg state, or form a Rydberg molecule. Both the atomic shift and the Rydberg molecule states depend on the initial internal state of the polar molecule, resulting in molecular state dependent van der Waals or dipole-dipole interaction between Rydberg atoms. Rydberg atoms mediated interaction between polar molecules can be enhanced up to 10(3) times. We describe how the coupling between a polar molecule and a Rydberg atom can be applied to coherently control molecular states, and specifically, to individually address molecules in an optical lattice, and to non-destructively readout molecular qubits.

Three body recombination of ultracold dipoles to weakly bound dimers.

We use universality in two-body dipolar physics to study three-body recombination. We present results for the universal structure of weakly bound two-dipole states that depend only on the s-wave scattering length (a). We study threshold three-body recombination rates into weakly bound dimer states as a function of the scattering length. A Fermi golden rule analysis is used to estimate rates for different events mediated by the dipole-dipole interaction and a phenomenological contact interaction. The three-body recombination rate in the limit where a≫D contains terms which scale as a{4}, a{2}D{2}, and D4, where D is the dipolar length. When a≪D, the three-body recombination rate scales as D4.

Ultracold giant polyatomic Rydberg molecules: coherent control of molecular orientation.

We predict the existence of a class of ultracold giant molecules formed from trapped ultracold Rydberg atoms and polar molecules. The interaction which leads to the formation of such molecules is the anisotropic, long-range charge-dipole interaction. We show that prominent candidate molecules such as deuterated hydroxyl (OD) and KRb should bind to Rydberg rubidium atoms, with energies E(b)≃5-25 GHz at distances R≃0.1-1 µm. These molecules form in double wells, mimicking chiral molecules, with each well containing a particular dipole orientation. We prepare a set of correlated dressed electron-dipole eigenstates which are used in an on-resonance Raman scheme to coherently control the molecular dipole orientation.

General theoretical description of N-body recombination.

Formulas for the cross section and event rate constant describing recombination of N particles are derived in terms of general S-matrix elements. Our result immediately yields the generalized Wigner threshold scaling for the recombination of N bosons. A semianalytical formula encapsulates the overall scaling with energy and scattering length, as well as resonant modifications by the presence of N-body states near the threshold collision energy in the entrance channel. We then apply our model to the case of four-boson recombination into an Efimov trimer and a free atom.

Collective coordinate description of anisotropically trapped degenerate Fermi gases.

The solution of the many-body Schrödinger equation using an adiabatic treatment of the hyperradius is generalized to treat two components of a hyperspherical vector adiabatically. This treatment has advantages in certain physical situations, such as the description of a degenerate Fermi gas or Bose-Einstein condensate in an anisotropic trapping potential. A first application to the zero-temperature anisotropic Fermi gas is compared with predictions of the Hartree-Fock method.

A homonuclear molecule with a permanent electric dipole moment.

Permanent electric dipole moments in molecules require a breaking of parity symmetry. Conventionally, this symmetry breaking relies on the presence of heteronuclear constituents. We report the observation of a permanent electric dipole moment in a homonuclear molecule in which the binding is based on asymmetric electronic excitation between the atoms. These exotic molecules consist of a ground-state rubidium (Rb) atom bound inside a second Rb atom electronically excited to a high-lying Rydberg state. Detailed calculations predict appreciable dipole moments on the order of 1 Debye, in excellent agreement with the observations.