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arXiv:2111.10013 · Physical Review Letters

Seconds-Scale Coherence on Nuclear Spin Transitions of Ultracold Polar Molecules in 3D Optical Lattices

Junyu Lin, J. He, Mucan Jin, Guanghua Chen, Dajun Wang

Published Jun 1, 2022• 30 citations
arXivHTMLPDF

Abstract

Ultracold polar molecules (UPMs) are emerging as a novel and powerful platform for fundamental applications in quantum science. Here, we report characterization of the coherence between nuclear spin levels of ultracold ground-state sodium-rubidium molecules loaded into a 3D optical lattice with a nearly photon scattering limited trapping lifetime of 9(1) seconds. After identifying and compensating the main sources of decoherence, we achieve a maximum nuclear spin coherence time of T_{2}^{*}=3.3(6) s with two-photon Ramsey spectroscopy. Furthermore, based on the understanding of the main factor limiting the coherence of the two-photon Rabi transition, we obtain a Rabi line shape with linewidth below 0.8 Hz. The simultaneous realization of long lifetime and coherence time, and ultrahigh spectroscopic resolution in our system unveils the great potentials of Ultracold polar molecules in quantum simulation, computation, and metrology.

DOI
10.1103/physrevlett.128.223201

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Ultracold polar molecules (UPMs) are emerging as a novel and powerful platform for fundamental applications in quantum science. Here, we report characterization of the coherence between nuclear spin levels of ultracold ground-state sodium-rubidium molecules loaded into a 3D optical lattice with a nearly photon scattering limited trapping lifetime of 9(1) seconds. After identifying and compensating the main sources of decoherence, we achieve a maximum nuclear spin coherence time of T_{2}^{*}=3.3(6) s with two-photon Ramsey spectroscopy. Furthermore, based on the understanding of the main factor limiting the coherence of the two-photon Rabi transition, we obtain a Rabi line shape with linewidth below 0.8 Hz. The simultaneous realization of long lifetime and coherence time, and ultrahigh spectroscopic resolution in our system unveils the great potentials of Ultracold polar molecules in quantum simulation, computation, and metrology.
Abstract Quantum states with long-lived coherence are essential for quantum computation, simulation and metrology. The nuclear spin states of ultracold molecules prepared in the singlet rovibrational ground state are an excellent candidate for encoding and storing quantum information. However, it is important to understand all sources of decoherence for these qubits, and then eliminate them, in order to reach the longest possible coherence times. Here, we fully characterise the dominant mechanisms for decoherence of a storage qubit in an optically trapped ultracold gas of RbCs molecules using high-resolution Ramsey spectroscopy. Guided by a detailed understanding of the hyperfine structure of the molecule, we tune the magnetic field to where a pair of hyperfine states have the same magnetic moment. These states form a qubit, which is insensitive to variations in magnetic field. Our experiments reveal an unexpected differential tensor light shift between the states, caused by weak mixing of rotational states. We demonstrate how this light shift can be eliminated by setting the angle between the linearly polarised trap light and the applied magnetic field to a magic angle of arccos(1/√3)≈55°. This leads to a coherence time exceeding 6.9 s (90% confidence level). Our results unlock the potential of ultracold molecules as a platform for quantum computation.
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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.
Highest-resolution laser spectroscopy has generally been limited to single trapped ion systems because of the rapid decoherence that plagues neutral atom ensembles. Precision spectroscopy of ultracold neutral atoms confined in a trapping potential now shows superior optical coherence without any deleterious effects from motional degrees of freedom, revealing optical resonance linewidths at the hertz level with a good signal-to-noise ratio. The resonance quality factor of 2.4 x 10(14) is the highest ever recovered in any form of coherent spectroscopy. The spectral resolution permits direct observation of the breaking of nuclear spin degeneracy for the 1S0 and 3P0 optical clock states of 87Sr under a small magnetic bias field. This optical approach for excitation of nuclear spin states allows an accurate measurement of the differential Landé g factor between 1S0 and 3P0. The optical atomic coherence demonstrated for collective excitation of a large number of atoms will have a strong impact on quantum measurement and precision frequency metrology.
This thesis presents the development of a toolbox for the coherent control of ultracold polar molecules. Such systems of molecules promise the creation of long-lived, highly dipolar quantum gases with applications spanning the fields of quantum state controlled chemistry, quantum information, quantum simulation, and precision measurement. However, the addition of vibrational and rotational degrees of freedom leads to molecular systems being significantly more complex than their widely used atomic counterparts. In this work we demonstrate full control of the quantum state down to the hyperfine level of an optically trapped sample of ultracold bosonic 87Rb133 Cs molecules, and exploit that control to begin an investigation into the collision processes which take place in an ultracold molecular gas. We create a sample of up to ∼ 4000 optically trapped molecules in their rovibronic and hyperfine ground state. We characterise the molecules by measuring their temperature, binding energy, and molecule-frame electric dipole moment. We perform spectroscopy of the first rotationally excited state with hyperfine state resolution using microwaves to determine accurate values of rotational and hyperfine coupling constants. We use coherent π pulses to perform complete transfer population between selected hyperfine levels of the ground, first-excited, and second-excited rotational states. We investigate the effect of the off-resonant light of our optical dipole trap on the rotational and hyperfine structure of the molecules. Through a combination of high-resolution microwave spectroscopy and parametric heating measurements, we characterise the polarisability of the 87Rb133Cs molecule. We demonstrate that coupling between neighbouring hyperfine states manifests in rich structure with many avoided crossings in any rotational state other than the ground state. This coupling may be tuned by rotating the polarisation of the linearly polarised trapping light. Finally, we study the lifetime of polar bosonic 87Rb133Cs molecules in our 3D optical dipole trap. We examine the lifetime of the molecules as a function of dipole trap intensity, magnetic field, and hyperfine and rotational state. Despite the chemical stability of the 87Rb133 Cs molecule, we observe lifetimes of ∼1 s corresponding to 2-body decay rates close to the universal limit.
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.