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arXiv:1702.00341 · Physical Review A

Anisotropic blockade using pendular long-range Rydberg molecules

Matthew T. Eiles, Hyun‐Woo Lee, Jesús Pérez‐Ríos, Chris H. Greene

Published May 30, 2017• 21 citations
arXivHTMLPDF

Abstract

We propose an experiment to demonstrate a blockade mechanism caused by long-range anisotropic interactions in an ultracold dipolar gas composed of the recently observed ``butterfly'' Rydberg molecules. At the blockade radius, the strong intermolecular interaction between two adjacent molecules shifts their molecular states out of resonance with the photoassociation laser, preventing their simultaneous excitation. When the molecules are prepared in a quasi-one-dimensional (Q1D) trap, the interaction's strength can be tuned via a weak external field. The molecular density thus depends strongly on the angle between the trap axis and the field. The available Rydberg and internal molecular states provide a wide range of tunability.

DOI
10.1103/physreva.95.052708

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Bulletin of the American Physical Society•Jun 9, 2017•0 citations
We propose an experiment to demonstrate a blockade mechanism caused by long-range anisotropic interactions in an ultracold dipolar gas composed of the recently observed ``butterfly'' Rydberg molecules. At the blockade radius, the strong intermolecular interaction between two adjacent molecules shifts their molecular states out of resonance with the photoassociation laser, preventing their simultaneous excitation. When the molecules are prepared in a quasi-one-dimensional (Q1D) trap, the interaction's strength can be tuned via a weak external field. The molecular density thus depends strongly on the angle between the trap axis and the field. The available Rydberg and internal molecular states provide a wide range of tunability.
Ultralong-range "butterfly" Rydberg molecules possess large dipole moments which lead to long-range anisotropic interactions between molecules. Their properties are studied using a Hamiltonian that fully includes the electronic and nuclear spin degrees of freedom. Using this more accurate and complete theoretical description, we investigate the intermolecular interaction when the molecules are prepared in pendular states. The anisotropy of this interaction manifests itself strongly in the density of created molecules.
Rydberg atoms have experimentally interestingproperties such as strong long-range Van der Waals interactions and the dipole blockade effect. In optical lattices the blockade effect ensures that only one Rydberg excitation per site is allowed, effectively creating a Rydberg crystal. We theoretically show that it is also possible for a one-dimensional Rydberg crystal to spontaneously form in a random ensemble of atoms, e.g. a magneto-optical trap. This is done using an existing Monte Carlo model [1] to simulate the excitation dynamics inside the intersection of two lasers for a two-step excitation scheme. With a blue-detuned laser for the upper transition, the first Rydberg excitation will occur after a relatively long time. That first Rydberg atom will then seed further Rydberg excitations, as the blockade effect shifts atoms at a certain distance into resonance. If two dimensions of the laser intersection are smaller than the blockade radius, a one-dimensional Rydberg crystal will form.
New phenomena have been observed by exciting ultracold ground-state atoms to Rydberg states. Starting with a dense sample of Rb atoms in a magneto-optical trap, we excite them to high Rydberg states (n = 30 - 90) with a single UV excitation pulse. Long-range molecular resonances with interatomic distances exceeding 104 a0 have been discovered. We have also observed the Rydberg excitation blockade, crucial for the implementation of quantum phase gates using neutral atoms. The physics behind these observations is attributed to the strong long-range van der Waals interactions among the Rydberg atoms. In addition, we have seen dipole (E1) forbidden but quadrupole (E2) allowed 5s → nd transitions, allowing us to determine the E2 oscillator strengths to these high Rydberg states. Our narrow-band UV pulsed laser system, with ∼100 MHz bandwidth, also allows us to measure the ratios of j-dependent oscillator strengths to the p and d Rydberg states. ^
Abstract We calculate pair potential curves for interacting Rydberg atoms in a constant electric field and use them to determine the effective C 3 dipole–dipole and C 6 van der Waals coefficients. We compare the C 3 and C 6 with experiments where the angle of a polarizing electric field is varied with respect to the axis of a quasi-1-dimensional trap at ultracold temperatures. The dipoles produced via polarization of the atoms have an angular dependent dipole–dipole interaction. We focus on the interaction potential of two rubidium Rydberg atoms in 50 S 1 / 2 states in the blockade regime. For internuclear distances close to the blockade radius, R bl ≈ 4–6 μ m, molecular calculations are in much better agreement with experimental results than those based on the properties of single atoms and independent calculations of C 3 and C 6 which were used to analyze the original experiment. We find that the calculated C 6 coefficient is within 8% of the experimental value while the C 3 coefficient is within 20% of the experimental value.
The creation of a gas of ultracold polar molecules with a high phase space density brings new possibilities beyond experiments with ultracold atomic gases. In particular, long-range, anisotropic, and tunable dipole-dipole interactions open the way for novel quantum gases, with applications including strongly correlated many-body systems, and ultracold chemistry. This thesis will present the final steps to complete control over both internal and external degrees of freedom of the molecule which allows us to control, and even completely suppress, the chemical reactions between molecules. First, the control over internal states has been achieved through coherent state transfer to the ro-vibronic ground state and coherent manipulations of the hyperfine and rotational states with microwave radiation. Second, external degrees of freedom are controlled by loading the gas into an optical lattice. With the molecules loaded into a one-dimensional lattice, the orientation of the molecular collisions is controlled by manipulating both internal (hyperfine states) and external (motional states in the direction of tight confinement) degrees of freedom. Most striking is that by preparing the molecules all in the lowest band of the lattice in the same internal state, the molecular collisions can only occur in a side-by-side" orientation, where the chemical reaction rate is suppressed by the repulsive dipole-dipole interactions. The chemical reaction can be suppressed completely by further constraining the motion in the trap in a strong 3D lattice. Here we see lifetimes longer than 20 s, limited by o-resonant light scattering. Finally, the ac polarizability of the molecules is explored and controlled. The different rotational states of the molecule have different polarizabilities and will experience a different trapping force in both the optical dipole trap or lattice. We show that there is a magic angle" between the quantization axis and the polarization of the trapping laser at which the polarizabilities of two different rotational states can be matched, eliminating dephasing and allowing for coherent manipulations between rotational states.
Rydberg atoms possess a strong atom-atom interaction, which limits its density in an atomic sample. Such effect is known as a Rydberg-atom blockade. Here, we present a way to control such effect by directly orienting the induced atomic dipole moment using a dc external electrical field. To demonstrate it, we excite the 50S1/250{S}_{1/2}50S1/2​ Rb atomic state in a quasiunidimensional sample held in a quasielectrostatic trap. A pure nSnSnS state holds only van der Waals interaction at long range, but in the presence of an external electric field the state mixing leads to strong dipole-dipole interactions. We have measured the Rydberg-atom population as a function of ground-state atoms density for several angles between the electric field and the main axis of the unidimensional sample. The results indicate that the limit on the final Rydberg density can be controlled by electric-field orientation. Besides, we have characterized the sample by using a single-atom ion imaging technique, demonstrating that it does behave as a unidimensional sample.