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.
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.
Arrays of trapped neutral atoms and polar molecules have separately emerged as powerful and complementary platforms for quantum science. Neutral atoms enable fast, programmable interactions through excitation to Rydberg states, whereas polar molecules possess long-lived rotational states that are attractive for quantum memories and qudits. Combining these platforms would create new possibilities, but requires a coherent interface between individual atoms and molecules, which so far has not been realised. Here, we establish such an interface between a single neutral atom and a single polar molecule. By tuning atomic and molecular transitions into resonance, we realise strong state-dependent dipolar interactions at micrometre separations in an optical tweezer platform with single-particle control. We exploit this interface to perform quantum operations between the two particles, demonstrating atom-mediated readout of a molecular qubit, coherent spin exchange, and entanglement using a blockade-based controlled-NOT operation. These results establish a new hybrid quantum platform at the intersection of atomic and molecular physics, in which long-lived molecular quantum information can be rapidly mapped onto an atom for readout or onward coherent transfer. The platform provides a route to hybrid quantum processors utilising atom-mediated readout and entanglement of molecular qubits, mixed-species quantum simulators of dipolar systems, and macroscopic entangled molecular states for quantum-enhanced metrology and precision sensing.
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.
We propose high-fidelity controlled-NOT (CNOT) gates in a hybrid system of polar molecules and Rydberg atoms based on the unconventional Rydberg pumping mechanism. By combining the rich internal structure of polar molecules with the strong dipole-dipole interactions of Rydberg atoms, we realize both two-to-one and one-to-two gate configurations. Numerical simulations show that the gate performance is robust against spontaneous emission from Rydberg states. The approach naturally extends to larger systems, as demonstrated by four-qubit implementations achieving three-to-one and one-to-three CNOT gates with fidelities exceeding 99\%. These results highlight hybrid molecule-Rydberg atom architectures as a promising platform for scalable quantum information processing.
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.
Ultracold polar molecules in optical lattices or tweezer arrays offer a promising platform for quantum information processing and simulation, thanks to their rich internal structure and long-range dipolar interactions. Recent experimental advances now allow precise control over individual molecules, enabling two-qubit gates based on the iSWAP gate. A key challenge is however the sensitivity to variations of the dipole-dipole interaction strength - stemming from motion of the molecules and uncertainty on the precise positioning of external confining potentials - that limits current gate fidelities. To address this, we develop a quantum optimal control framework, based on a perturbative approach, to design gates that are robust with respect to quasi-static deviations of Hamiltonian parameters, and provide criteria to evaluate a priori whether a gate can be made robust for a given control Hamiltonian. By applying these criteria to exchange-coupled qubits, as polar molecules, we demonstrate that robustness cannot be achieved with global controls only, but can be attained by breaking the exchange symmetry through local controls, such as a local detuning. We determine the robust time-optimal solution for realizing an iSWAP gate, show that the control pulses can be designed to be smooth functions, and achieve theoretical gate fidelities compatible with error correction under realistic parameters. Additionally, we show that certain entangled state preparations, such as Bell states, can be made robust even with global controls only. We demonstrate that, under the adiabatic approximation - where molecular motion occurs on timescales faster than that of the exchange interaction - the noise arising from thermal motion can be effectively treated as quasi-static variations of Hamiltonian parameters. This allows us to extend our treatment to the concrete experimental case of polar molecules.
The challenge of building a scalable quantum processor requires consolidation of the conflicting requirements of achieving coherent control and preservation of quantum coherence in a large scale quantum system. Moreover, the system should be compatible with miniaturization and integration of quantum circuits. Mesoscopic solid state systems such as superconducting islands and quantum dots feature robust control techniques using local electrical signals and self-evident scaling based on advances in fabrication; however, in general the quantum states of solid state devices tend to decohere rapidly. In contrast, quantum optical systems based on trapped ions and neutral atoms exhibit dramatically better coherence properties, while miniaturization of atomic and molecular systems, and their integration with mesoscopic electrical circuits, remains an important challenge. Below we describe methods for the integration of a single particle system -- an isolated polar molecule -- with mesoscopic solid state devices in a way that produces robust, coherent, quantum-level control. The methods described include the trapping, cooling, detection, coherent manipulation and quantum coupling of isolated polar molecules at sub-micron dimensions near cryogenic stripline microwave resonators. We show that electrostatically trapped polar molecules can exhibit strong confinement and fast, purely electrical gate control. Furthermore, the effect of electrical noise sources, a key issue in quantum information processing, can be suppressed to very low levels via appropriate preparation and manipulation of the polar molecules. Our setup provides a scalable cavity QED-type quantum computer architecture, where entanglement of distant qubits stored in long-lived rotational molecular states is achieved via exchange of microwave photons.