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.
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.
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.
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.
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.
Polar molecules in superpositions of rotational states exhibit long-range dipolar interactions, but maintaining their coherence in a trapped sample is a challenge. We present calculations that show many laser-coolable molecules have convenient rotational transitions that are exceptionally insensitive to magnetic fields. We verify this experimentally for CaF where we find a transition with sensitivity below 5 Hz G^{-1} and use it to demonstrate a rotational coherence time of 6.4(8) ms in a magnetic trap. Simulations suggest it is feasible to extend this to more than 1 s using a smaller cloud in a biased magnetic trap.
Ultracold quantum gases are versatile model systems for exploring quantum physics or for the simulation of solid state materials. Meanwhile, they have been created from various atomic species - from alkali metals over alkaline earths to rare earth elements. The latest addition are quantum gases of different kinds of polar molecules. Expectations for quantum gases of heteronuclear molecules are high: Due to their large electric dipole moments, these molecules can interact with each other via long-range interactions - not just via contact interactions as is the case for most atoms. Additionally, they have vibrational and rotational degrees of freedom, with open up new possibilities for quantum simulation. But the same degrees of freedom also pose some challenges. For example, they make the preparation of the quantum gas more difficult, which is typically produced with a combination of laser cooling and evaporative cooling in the atomic case. Molecules mostly lack closed transitions in their spectra, which are required for laser cooling. Therefore, we create our molecular quantum gas from a mixture of two atomic quantum gases. In this work, such an experimental method was developed for fermionic NaK molecules, which is based on the two-photon process Stimulated Raman Adiabatic Passage (STIRAP). Within STIRAP, the hyperfine structure of the chosen intermediate state plays an important role. Experimentally, and with the help of a theoretical model describing the whole process, we find that we produce the most molecules when we use a large one-photon detuning, if the hyperfine structure of the intermediate state is unresolved. In another project, we explored the rotational level structure of the molecular ground state populated by STIRAP. Rotation is closely linked to the electric dipole moment. The superposition of the ground state with the first excited rotational state, for example, has a transition dipole moment of almost 60% of the permanent electric dipole moment. Unfortunately, coherence times of such superpositions are typically short, as the different polarizabilities of the rotational states lead to dephasing in optical traps. However, using a special polarization angle and a small, dc electric field, we can compensate these differences and realize a spin-decoupled magic trap. With this new technique we obtain record coherence times, at least for small molecular densities. For larger densities we observe first indications for dipolar interactions in a bulk gas of polar molecules, which we also model using the moving-average cluster expansion (MACE).
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.