Hybrid quantum systems offer a route to combining the complementary strengths of distinct quantum platforms while mitigating their limitations. A particularly promising architecture combines neutral atoms and polar molecules: atoms provide fast, controllable interactions through excitation to Rydberg states, while molecules possess long-lived rotational states that are attractive for quantum memories and qudits. Although dipolar interactions between atoms and molecules have been observed in gas-phase and beam experiments, they have not previously been explored in a scalable optical tweezer platform that enables the controlled coherent interactions needed for quantum state transfer and entanglement. Here, we realise this goal, demonstrating coherent dipolar interactions between an individual Rydberg atom and an individual polar molecule. The separation of the particles is controlled using species-specific optical tweezers and their dipolar interactions are made strongly state-dependent by tuning two atom-molecule pair states into resonance. We exploit these interactions to demonstrate atom-mediated state readout of a molecular qubit, observe coherent spin exchange between the particles, and generate entanglement using a blockade-based controlled-NOT operation. Together, these results establish a coherent atom-molecule interface in which long-lived molecular quantum information can be rapidly mapped onto internal states of a Rydberg atom for readout or onward coherent transfer. This platform can be scaled to realise hybrid quantum processors utilising atom-mediated readout and entanglement of molecular qubits and mixed-species quantum simulators of dipolar systems.
Hybrid quantum systems offer a route to combining the complementary strengths of distinct quantum platforms while mitigating their limitations. A particularly promising architecture combines neutral atoms and polar molecules: atoms provide fast, controllable interactions through excitation to Rydberg states, while molecules possess long-lived rotational states that are attractive for quantum memories and qudits. Although dipolar interactions between atoms and molecules have been observed in gas-phase and beam experiments, they have not previously been explored in a scalable optical tweezer platform that enables the controlled coherent interactions needed for quantum state transfer and entanglement. Here, we realise this goal, demonstrating coherent dipolar interactions between an individual Rydberg atom and an individual polar molecule. The separation of the particles is controlled using species-specific optical tweezers and their dipolar interactions are made strongly state-dependent by tuning two atom-molecule pair states into resonance. We exploit these interactions to demonstrate atom-mediated state readout of a molecular qubit, observe coherent spin exchange between the particles, and generate entanglement using a blockade-based controlled-NOT operation. Together, these results establish a coherent atom-molecule interface in which long-lived molecular quantum information can be rapidly mapped onto internal states of a Rydberg atom for readout or onward coherent transfer. This platform can be scaled to realise hybrid quantum processors utilising atom-mediated readout and entanglement of molecular qubits and mixed-species quantum simulators of dipolar systems.
We show that an array of polar molecules interacting with Rydberg atoms is a promising hybrid system for scalable quantum computation.Quantum information is stored in long-lived hyperfine or rotational states of molecules, which interact indirectly through resonant dipole-dipole interactions with Rydberg atoms.A two-qubit gate based on this interaction has a duration of 1 μs and an achievable fidelity of 99.9%.The gate has little sensitivity to the motional states of the particles-the molecules can be in thermal states, the atoms do not need to be trapped during Rydberg excitation, the gate does not heat the molecules, and heating of the atoms has a negligible effect.Within a large, static array, the gate can be applied to arbitrary pairs of molecules separated by tens of micrometres, making the scheme highly scalable.The molecule-atom interaction can also be used for rapid qubit initialization and efficient, nondestructive qubit readout, without driving any molecular transitions.Single-qubit gates are driven using microwave pulses alone, exploiting the strong electric dipole transitions between rotational states.Thus, all operations required for large-scale quantum computation can be done without moving the molecules or exciting them out of their ground electronic states.
Hybrid quantum systems combining neutral atoms and trapped ions offer the prospect of integrating the scalability of atom arrays with the high-fidelity control available in trapped-ion platforms. Here we propose and analyze a quantum interface between individually trapped neutral atoms and a trapped-ion crystal. In our scheme, a neutral 88Sr atom trapped in optical tweezers interacts with a small 88Sr+ ion crystal, and by exciting the atom to a Rydberg state, the atom-ion polarization interaction is strongly enhanced, resulting in a state-dependent modification of the ions' collective motional modes. We show that this shift enables conditional control of a MS gate, allowing the neutral atom to act as a control qubit for an entangling operation between two ions. We investigate the feasibility of the scheme by analyzing Rydberg trapping in the combined optical tweezers and Paul trap potentials, identifying negative-polarizability Rydberg states as particularly favorable for stable confinement. We further evaluate the relevant trapping conditions, Rydberg lifetimes, and coherence requirements, and show that the proposed interface is compatible with realistic experimental parameters. These results establish a practical route toward deterministic atom-ion hybrid quantum gates and quantum interfaces.
Polar molecules, with their rich internal structure, offer immense potential for fundamental physics, quantum technology, and controlled chemistry. However, their utilization is currently limited because of slow and imperfect state detection and weak dipolar interaction, limiting fast and large-scale entanglement generation. We propose and analyze a scheme for quantum logic control and measurement-based state preparation in a hybrid platform of polar molecules and neutral atoms. The method leverages fast, high-fidelity atom-molecule gates and high-fidelity atomic ancilla measurements to overcome the common challenges in molecule-only platforms, while preserving their diverse structural advantages. The proposed atom-molecule controlled-phase gate is based on resonant dipole-dipole exchange between a molecular rotational transition and an atomic Rydberg transition, rendering it three orders of magnitude faster than any direct molecule-molecule entangling gate. We further study several applications of our scheme including the preparation of molecular GHZ states for quantum enhanced precision measurements, the preparation of exotic molecular qudit states with topological order, and measurement-altered criticality. Our scheme is applicable to any polar molecule. It expands the paradigm of quantum logic control and paves the way to large-scale molecular entangled states. More generally, it highlights a concrete hybrid quantum system in which each qubit is utilized in an optimal way and where the measurement-based approach can yield a significant advantage in near-term devices.
Models of interacting quantum spins are used in many areas of physics ranging from the study of magnetism and strongly correlated materials to quantum sensing. In this work, we study coherent many-body dynamics of interacting spin models realized using polar molecules trapped in rearrangeable optical tweezer arrays. Specifically, we encode quantum spins in long-lived rotational states and use the electric dipolar interaction between molecules, together with Floquet Hamiltonian engineering, to realize 1/r3 XXZ and XYZ models. We microscopically probe several types of coherent dynamics in these models, including quantum walks of single spin excitations, the emergence of magnon bound states, and coherent creation and annihilation of magnon pairs. Our results establish molecular tweezer arrays as a new quantum simulation platform for interacting quantum spin models.
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.
The ability to control particles in the quantum regime at the individual particle level is a challenge at the frontier of quantum science and engineering. Of the many quantum objects developed in pursuit of this goal, ultracold molecules host rich internal states and unique inter-particle interactions that could lend themselves useful to a broad range of applications including quantum computing and simulation, precision measurements and quantum chemistry. In this thesis we present a bottom-up approach to creating single molecules in individual optical tweezers. In particular, single atoms of two different species are first trapped and cooled in individual optical tweezers then brought together to form a single molecule coherently. Using this approach, we have successfully created an array of fully quantum-state-controlled polar molecules. The quantum state – including both internal and external states – of the resulting molecules are known to us, and is the first time single neutral molecules have been under full quantum state control. This platform offers exciting new opportunities to harness the rich properties of molecules in many quantum science applications.