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arXiv:2306.07264 · Physical Review Letters

Extended Rotational Coherence of Polar Molecules in an Elliptically Polarized Trap

Annie Jihyun Park, Lewis R. B. Picard, Gabriel E. Patenotte, Jessie T. Zhang, Till Rosenband, Kang-Kuen Ni

Published Oct 30, 2023• 21 citations
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Abstract

We demonstrate long rotational coherence of individual polar molecules in the motional ground state of an optical trap. In the present, previously unexplored regime, the rotational eigenstates of molecules are dominantly quantized by trapping light rather than static fields, and the main source of decoherence is differential light shift. In an optical tweezer array of NaCs molecules, we achieve a three-orders-of-magnitude reduction in differential light shift by changing the trap's polarization from linear to a specific "magic" ellipticity. With spin-echo pulses, we measure a rotational coherence time of 62(3) ms (one pulse) and 250(40) ms (up to 72 pulses), surpassing the projected duration of resonant dipole-dipole entangling gates by orders of magnitude.

DOI
10.1103/physrevlett.131.183401

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We demonstrate long rotational coherence of individual polar molecules in the motional ground state of an optical trap. In the present, previously unexplored regime, the rotational eigenstates of molecules are dominantly quantized by trapping light rather than static fields, and the main source of decoherence is differential light shift. In an optical tweezer array of NaCs molecules, we achieve a three-orders-of-magnitude reduction in differential light shift by changing the trap's polarization from linear to a specific "magic" ellipticity. With spin-echo pulses, we measure a rotational coherence time of 62(3) ms (one pulse) and 250(40) ms (up to 72 pulses), surpassing the projected duration of resonant dipole-dipole entangling gates by orders of magnitude.
Qubit coherence times are critical to the performance of any robust quantum computing platform. For quantum information processing using arrays of polar molecules, a key performance parameter is the molecular rotational coherence time. We report a 93(7) ms coherence time for rotational state qubits of laser cooled CaF molecules in optical tweezer traps, over an order of magnitude longer than previous systems. Inhomogeneous broadening due to the differential polarizability between the qubit states is suppressed by tuning the tweezer polarization and applied magnetic field to a "magic" angle. The coherence time is limited by the residual differential polarizability, implying improvement with further cooling. A single spin-echo pulse is able to extend the coherence time to nearly half a second. The measured coherence times demonstrate the potential of polar molecules as high fidelity qubits.
Superpositions of rotational states in polar molecules induce strong, long-range dipolar interactions. Here we extend the rotational coherence by nearly 1 order of magnitude to 8.7(6) ms in a dilute gas of polar ^{23}Na^{40}K molecules in an optical trap. We demonstrate spin-decoupled magic trapping, which cancels first-order and reduces second-order differential light shifts. The latter is achieved with a dc electric field that decouples nuclear spin, rotation, and trapping light field. We observe density-dependent coherence times, which can be explained by dipolar interactions in the bulk gas.
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.
Abstract Ultracold polar molecules combine a rich structure of long-lived internal states with access to controllable long-range anisotropic dipole–dipole interactions. In particular, the rotational states of polar molecules confined in optical tweezers or optical lattices may be used to encode interacting qubits for quantum computation or pseudo-spins for simulating quantum magnetism. As with all quantum platforms, the engineering of robust coherent superpositions of states is vital. However, for optically trapped molecules, the coherence time between rotational states is typically limited by inhomogeneous differential light shifts. Here we demonstrate a rotationally magic optical trap for 87 Rb 133 Cs molecules that supports a Ramsey coherence time of 0.78(4) s in the absence of dipole–dipole interactions. This is estimated to extend to >1.4 s at the 95% confidence level using a single spin-echo pulse. In our trap, dipolar interactions become the dominant mechanism by which Ramsey contrast is lost for superpositions that generate oscillating dipoles. By changing the states forming the superposition, we tune the effective dipole moment and show that the coherence time is inversely proportional to the strength of the dipolar interaction. Our work unlocks the full potential of the rotational degree of freedom in molecules for quantum computation and quantum simulation.
Rotational states of ultracold polar molecules possess long lifetimes, microwave-domain coupling, and tunable dipolar interactions. The availability of numerous rotational states has inspired many applications, including simulating quantum magnetism, encoding high-dimensional qudits and generating large synthetic dimensions. However, engineering the coherent superpositions of multiple rotational states needed for these applications is difficult owing to strong differential light shifts. Here, we overcome this challenge using individual molecules confined in near-magic wavelength optical tweezers. Through precision Ramsey spectroscopy, we find the exact magic wavelengths and sensitivities to detuning errors for multiple rotational state superpositions. We find for traps polarised parallel to the quantisation axis, the magic wavelengths are closely clustered enabling long-lived coherence across multiple rotational states simultaneously. Using a generalised Ramsey sequence, we demonstrate second-scale coherent spin-1 dynamics encoded in three rotational states and perform multiparameter estimation. With modest experimental improvements, we predict second-scale coherence across ten rotational states is achievable.