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arXiv:2012.09043 · Physical Review X

Coherent Optical Creation of a Single Molecule

Yichao Yu, Kenneth Wang, Jonathan D. Hood, Lewis R. B. Picard, Jessie T. Zhang, William B. Cairncross, Jeremy M. Hutson, Rosario González‐Férez, Till Rosenband, Kang-Kuen Ni

Published Sep 17, 2021• 26 citations
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Abstract

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.

DOI
10.1103/physrevx.11.031061

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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 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 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 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.
Abstract We present a study of two-photon pathways for the transfer of NaCs molecules to their rovibrational ground state. Starting from NaCs Feshbach molecules, we perform bound-bound excited state spectroscopy in the wavelength range from 900 nm to 940 nm, covering more than 30 vibrational states of the c 3 Σ + , b 3 Π , and B 1 Π electronic states. Analyzing the rotational substructure, we identify the highly mixed c 3 Σ 1 + | v = 22 ⟩ ∼ b 3 Π 1 | v = 54 ⟩ state as an efficient bridge for stimulated Raman adiabatic passage. We demonstrate transfer into the NaCs ground state with an efficiency of up to 88(4)%. Highly efficient transfer is critical for the realization of many-body quantum phases of strongly dipolar NaCs molecules and high fidelity detection of single molecules, for example, in spin physics experiments in optical lattices and quantum information experiments in optical tweezer arrays.
One possibility for the creation of ultracold, high phase space density quantum gases of molecules in the rovibronic ground state relies on first associating weakly-bound molecules from quantum-degenerate atomic gases on a Feshbach resonance and then transferring the molecules via several steps of coherent two-photon stimulated Raman adiabatic passage (STIRAP) into the rovibronic ground state. Here, in ultracold samples of Cs2 Feshbach molecules produced out of ultracold samples of Cs atoms, we observe several optical transitions to deeply-bound rovibrational levels of the excited 0(u)+ molecular potentials with high resolution. At least one of these transitions, although rather weak, allows efficient STIRAP transfer into the deeply-bound vibrational level (see text for symbols)v = 73 > of the singlet X1 sigma(g)+ ground state potential, as recently demonstrated (J. G. Danzl, E. Haller, M. Gustavsson, M. J. Mark, R. Hart, N. Bouloufa, O. Dulieu, H. Ritsch, and H.-C. Nägerl, Science, 2008, 321, 1062). From this level, the rovibrational ground state (see text for symbols)v = 0, J = 0 > can be reached with one more transfer step. In total, our results show that coherent ground state transfer for Cs2 is possible using a maximum of two successive two-photon STIRAP processes or one single four-photon STIRAP process.
Using the technique of stimulated Raman adiabatic passage (STIRAP) we have coherently transferred ultracold (87)Rb(2) Feshbach molecules into a more deeply bound vibrational quantum level. Our measurements indicate a high transfer efficiency of up to 87%. Because the molecules are held in an optical lattice with not more than a single molecule per lattice site, inelastic collisions between the molecules are suppressed and we observe long molecular lifetimes of about 1 s. Using STIRAP we have created quantum superpositions of the two molecular states and tested their coherence interferometrically. These results represent an important step towards Bose-Einstein condensation of molecules in the vibrational ground state.