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arXiv:2003.07850 · Physical Review Letters

Forming a Single Molecule by Magnetoassociation in an Optical Tweezer

Jessie T. Zhang, Yichao Yu, William B. Cairncross, Kenneth Wang, Lewis R. B. Picard, Jonathan D. Hood, Yen-Wei Lin, Jeremy M. Hutson, Kang-Kuen Ni

Published Jun 25, 2020• 71 citations
arXivHTMLPDF

Abstract

We demonstrate the formation of a single NaCs molecule in an optical tweezer by magnetoassociation through an s-wave Feshbach resonance at 864.11(5) G. Starting from single atoms cooled to their motional ground states, we achieve conversion efficiencies of 47(1)%, and measure a molecular lifetime of 4.7(7) ms. By construction, the single molecules are predominantly [77(5)%] in the center-of-mass motional ground state of the tweezer. Furthermore, we produce a single p-wave molecule near 807 G by first preparing one of the atoms with one quantum of motional excitation. Our creation of a single weakly bound molecule in a designated internal state in the motional ground state of an optical tweezer is a crucial step towards coherent control of single molecules in optical tweezer arrays.

DOI
10.1103/physrevlett.124.253401

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•May 21, 2019•1 citation
We demonstrate the formation of a single NaCs molecule in an optical tweezer by magnetoassociation through an s-wave Feshbach resonance at 864.11(5) G. Starting from single atoms cooled to their motional ground states, we achieve conversion efficiencies of 47(1)%, and measure a molecular lifetime of 4.7(7) ms. By construction, the single molecules are predominantly [77(5)%] in the center-of-mass motional ground state of the tweezer. Furthermore, we produce a single p-wave molecule near 807 G by first preparing one of the atoms with one quantum of motional excitation. Our creation of a single weakly bound molecule in a designated internal state in the motional ground state of an optical tweezer is a crucial step towards coherent control of single molecules in optical tweezer arrays.
We demonstrate the coherent creation of a single NaCs molecule in its rotational, vibrational, and electronic (rovibronic) ground state in an optical tweezer. Starting with a weakly bound Feshbach molecule, we locate a two-photon transition via the |c^{3}Σ_{1},v^{'}=26⟩ excited state and drive coherent Rabi oscillations between the Feshbach state and a single hyperfine level of the NaCs rovibronic ground state |X^{1}Σ,v^{''}=0,N^{''}=0⟩ with a binding energy of D_{0}=h×147044.63(11) GHz. We measure a lifetime of 3.4±1.6 s for the rovibronic ground state molecule, which possesses a large molecule-frame dipole moment of 4.6D and occupies predominantly the motional ground state. These long-lived, fully quantum-state-controlled individual dipolar molecules provide a key resource for molecule-based quantum simulation and information processing.
We report coherent association of atoms into a single weakly bound NaCs molecule in an optical tweezer through an optical Raman transition.The Raman technique uses a deeply bound electronic excited intermediate state to achieve a large transition dipole moment while reducing photon scattering.Starting from two atoms in their relative motional ground state, we achieve an optical transfer efficiency of 69%.The molecules have a binding energy of 770.2 MHz at 8.83(2) G.This technique does not rely on Feshbach resonances or narrow excited-state lines and may allow a wide range of molecular species to be assembled atom by atom.
We demonstrate the formation of a single RbCs molecule during the merging of two optical tweezers, one containing a single Rb atom and the other a single Cs atom. Both atoms are initially predominantly in the motional ground states of their respective tweezers. We confirm molecule formation and establish the state of the molecule formed by measuring its binding energy. We find that the probability of molecule formation can be controlled by tuning the confinement of the traps during the merging process, in good agreement with coupled-channel calculations. We show that the conversion efficiency from atoms to molecules using this technique is comparable to magnetoassociation.
We demonstrate full quantum state control of two species of single atoms using optical tweezers and assemble the atoms into a molecule.Our demonstration includes 3D ground-state cooling of a single atom (Cs) in an optical tweezer, transport by several microns with minimal heating, and merging with a single Na atom.Subsequently, both atoms occupy the simultaneous motional ground state with 61(4)% probability.This realizes a sample of exactly two cotrapped atoms near the phase-space-density limit of one, and allows for efficient stimulated-Raman transfer of a pair of atoms into a molecular bound state of the triplet electronic ground potential a 3 Σ þ .The results are key steps toward coherent creation of single ultracold molecules for future exploration of quantum simulation and quantum information processing.
Ultracold polar molecules possess a manifold of long-lived molecular rotational states, which can be coherently controlled using microwave fields and entangled by the long-range dipole-dipole interactions between molecules. The ability to control these features at the individual molecule level provides a rich toolbox with which to engineer quantum simulations of exotic materials or build a molecular quantum computer. Until recently, this level of single molecule control has eluded researchers due to the challenges inherent in taming the complex internal structure of molecules. In this thesis, we demonstrate full control over the internal quantum states and coherent interactions of individual NaCs molecules in optical tweezers. This platform is based on coherent assembly of ultracold Na and Cs atoms trapped and cooled in separate arrays, before being magnetoassociated at a Feshbach resonance to form weakly-bound molecules. Using high-resolution spectroscopy of electronically excited molecular states, we identify an efficient two-photon pathway to the rovibrational ground state of NaCs that we use to prepare an array of ground state molecules in tweezers. We demonstrate a "magic ellipticity'' technique to eliminate differential light shifts between two molecular rotational states and achieve coherence times of up to 250(40) ms for a superposition of those states. We then show that we can rearrange molecules in an array to eliminate defects and perform single-shot readout of multiple rotational states using controlled molecule dissociation and imaging of constituent atoms at high magnetic field. Finally, we coherently control the dipole-dipole interactions between two molecules, producing a Bell state with a fidelity of 94(3) % and demonstrating a universal entangling iSWAP gate for qubits encoded in molecular hyperfine states.
Recent theoretical and experimental advances have led to better understanding and control of simple molecules, bringing them to the forefront of quantum science. Diatomic polar molecules, with their vibrational and rotational degrees of freedom and electric dipole moment, are excellent candidates for a scalable qubit, probes of beyond-Standard Model physics, and quantum simulation of topological and chiral many-body systems. These applications call for high-phase space density (PSD) of molecules in a single quantum state. To date, the highest molecular PSD is achieved by coherently associating degenerate quantum gases of atoms into molecules. However, this requires fine-tuning of experimental parameters to maximize spatial overlap of the atomic density distributions while minimizing three-body recombination of the atoms.\nIn this thesis, we propose a bottom-up solution to gain single particle control of ultracold molecules for the first time. We use optical tweezers to deterministically assemble a single NaCs molecule in a single quantum state from a pair of Na and Cs atoms. Added benefits of using optical tweezers include: tight confinement of isolated atoms enabling cooling of Na and Cs to their quantum ground state of motion in less than 100~ms, and dynamic reconfigurability of optical tweezer arrays which will allow scaling up to defect-free arrays of single molecules. In the process, we realize a conceptually simple platform for studying atomic collisions and molecular spectra which derives its strength from the ability to gather "before" and "after" images of single atoms.