molecule NaCs, utilizing a pair of nuclear spin states as storage qubits. A third rotationally excited state with rotation-hyperfine coupling enables switchable electric dipolar exchange interactions between two molecules to generate an iSWAP gate. All three states are insensitive to external magnetic and electric fields. Impacts on gate fidelity due to coupling to other molecular states, imperfect ground-state cooling, blackbody radiation and vacuum spontaneous emission are small, leading to potential fidelity above 99.99% in a coherent quantum system that can be scaled by purely optical means.
molecule NaCs, utilizing a pair of nuclear spin states as storage qubits. A third rotationally excited state with rotation-hyperfine coupling enables switchable electric dipolar exchange interactions between two molecules to generate an iSWAP gate. All three states are insensitive to external magnetic and electric fields. Impacts on gate fidelity due to coupling to other molecular states, imperfect ground-state cooling, blackbody radiation and vacuum spontaneous emission are small, leading to potential fidelity above 99.99% in a coherent quantum system that can be scaled by purely optical means.
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.
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.
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.
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.
Proposals for quantum computing using rotational states of polar molecules as qubits have previously considered only diatomic molecules. For these the Stark effect is second-order, so a sizable external electric field is required to produce the requisite dipole moments in the laboratory frame. Here we consider use of polar symmetric top molecules. These offer advantages resulting from a first-order Stark effect, which renders the effective dipole moments nearly independent of the field strength. That permits use of much lower external field strengths for addressing sites. Moreover, for a particular choice of qubits, the electric dipole interactions become isomorphous with NMR systems for which many techniques enhancing logic gate operations have been developed. Also inviting is the wider chemical scope, since many symmetric top organic molecules provide options for auxiliary storage qubits in spin and hyperfine structure or in internal rotation states.
Optically trapped ultracold polar molecules can have multiple long-lived states for coding quantum information, and can exhibit electric dipole-dipole interactions~(DDI) which enables entanglement generation. The general understanding on the quantized motion~(QM) of molecules in the traps is that it causes fluctuation of DDI. Here, we find that the molecular QM can realize an asymmetric quantum Rabi model, which is of specific importance in the study of fundamental physics. The molecular QM can also lead to an exotic trap-dipole resonance, resulting in excess population loss to uncoupled motional states, and, hence, should be avoided in a general quantum control over polar molecules. To examine the impact of QM on quantum computing based on polar molecules, we introduce two gate protocols, a fast iSWAP gate which can be realized by a global microwave pulse of pulse area smaller than 2π, and a controlled-phase gate with an arbitrary controlled phase, and find that both gates can attain a high fidelity.