Polar molecules are a promising platform for quantum-enhanced sensing and precision tests of fundamental physics, owing to their strong long-range dipolar interactions, broad sensitivity to electromagnetic fields, and sensitivity to potential physics beyond the Standard Model. However, the creation of metrologically useful entangled states in molecular systems has remained elusive. Here, we report the first observation of a class of metrologically useful entangled states - spin-squeezed states - in polar CaF molecules trapped in an optical tweezer array. The spin degree of freedom is encoded in rotational levels which are directly coupled by dipolar exchange interactions. By harnessing appropriate dynamical decoupling schemes we observe up to 3.0(3)dB of metrological gain, (2.2(3)dB without measurement correction) from direct exchange interactions. Using Floquet engineering, we further realize richer Hamiltonians that preserve spin squeezing while enabling the development of longer-range quantum correlations. Using site- and spin-resolved measurements we demonstrate that these entangled states enhance sensitivity to both homogeneous and spatially varying fields, and reveal strong non-classical correlations, including bipartite entanglement and Einstein-Podolsky-Rosen steering. Finally, we transfer the spin-squeezed states into long-lived and non-interacting hyperfine states, where the metrological enhancement persists for up to 100ms. Our results establish molecular optical tweezer arrays as a scalable platform for generating, controlling, characterizing, and storing entangled states of molecules, opening new opportunities for quantum-enhanced sensing and precision tests of fundamental physics.
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 are promising candidate qubits for quantum computing and quantum simulations. Their long-lived molecular rotational states form robust qubits, and the long-range dipolar interaction between molecules provides quantum entanglement. In this work, we demonstrate dipolar spin-exchange interactions between single calcium monofluoride (CaF) molecules trapped in an optical tweezer array. We realized the spin-[Formula: see text] quantum XY model by encoding an effective spin-[Formula: see text] system into the rotational states of the molecules and used it to generate a Bell state through an iSWAP operation. Conditioned on the verified existence of molecules in both tweezers at the end of the measurement, we obtained a Bell state fidelity of 0.89(6). Using interleaved tweezer arrays, we demonstrate single-site molecular addressability.
Ultracold molecules are attractive candidates for various applications including ultracold chemistry, quantum information processing, quantum simulation and searches for physics beyond the standard model. Combined with optical tweezer techniques, an optical tweezer array of ultracold polar molecules holds promise for versatile quantum applications. Their long-lived molecular rotational states form robust qubits, while the long-range dipolar interaction between molecules provides quantum entanglement. In this thesis, we build a new generation experiment of optical tweezer array of ultracold CaF molecules. We optically transport the laser cooled and optically trapped molecules into a science glass cell using a hybrid method, where high numerical aperture optical access allows for tighter optical tweezers. In an array of these tight optical tweezers, we demonstrate dipolar spin-exchange interactions between single CaF molecules for the first time. We realize the spin-
21 quantum XY model by encoding an effective spin-
21 system into the rotational states of the molecules, and use it to generate a Bell state through an iSWAP operation. Conditioned on the verified existence of molecules in both tweezers at the end of the measurement, we obtain a Bell state fidelity of 0.89(6). Employing interleaved tweezer arrays, we demonstrate single site molecular addressability. To further improve the platform, cooling of the molecules to near the motional ground state is crucial for reducing various dephasings. We demonstrate Raman sideband cooling (RSC) of CaF molecules in optical tweezers to near their 3-D motional ground state, with a 3-D motional ground state probability of
54±18% of the molecules that survive the RSC. This paves the way to increase molecular coherence times in optical tweezers for robust quantum information processing and simulation applications in the near future.
Ultracold polar molecules provide a powerful platform for quantum science because they combine long-lived rotational states, rich internal structure, and strong electric dipole-dipole interactions. Optical tweezer arrays provide a pristine way of controlling these molecules at single-particle level, in which molecules can be individually trapped, rearranged into programmable geometries, coherently manipulated by optical and microwave fields, and entangled through their native dipolar interactions. This dissertation describes the development of geometric control as a resource for improving interaction coherence and high fidelity of quantum entanglement between directly laser-cooled calcium monofluoride (CaF) molecules in optical tweezers. A central challenge in molecular tweezer systems is that dipolar interactions are intrinsically sensitive to the relative position of the molecules. Thermal motion in the traps, especially along the weakly confined axial direction, causes molecules to sample a distribution of intermolecular separations, degrading dipolar coherence and limiting entanglement fidelity. We show in this work that the interaction itself can be made robust by controlling its geometry. The experimental work begins with improvements to the production and optical trapping of dense CaF samples. We realize a blue-detuned ``conveyor-belt" magneto-optical trap (MOT) that compresses laser-cooled CaF to a mean cloud radius of
64(5) μm and a peak density of
3.6(5)×1010 cm−3, a 600-fold density increase over conventional red-detuned CaF MOTs. Loading from this compressed source into an optical dipole trap yields up to
2.6×104 trapped molecules at
14(2) μK, with a peak phase-space density of approximately
2.4×10−6. This high-density source improves the transfer of laser-cooled molecules into conservative optical traps and provides the starting point for loading and manipulating single molecules in a hybrid SLM-AOD optical tweezer array. Using this platform, we prepare CaF molecules in selected rotational and hyperfine states to encode a rotational qubiyt. We show how to preserve the single-qubit coherence with a combination of techniques, including ``magic" polarization condition and microwave dynamical decoupling, as well as reduce motional quantum state of the trapped molecule with Raman sideband cooling. We then characterize coherent dipolar spin exchange between pairs of molecules and identify thermal motion and relative trap-center offsets as dominant sources of interaction dephasing. To suppress these effects, we engineer the three-dimensional interaction geometry between two individually trapped molecules. More specifically, we show that one can tune the \textit{static} geometric of the dipolar interaction to configurations where sensitivity to thermal fluctuations is strongly reduced while retaining a finite interaction strength. Furthermore, we show that a molecule can be moved during the interaction while preserving the coherence of ongoing entangling operations. We leverage programmable molecular motion to refocus dephasing arising from relative positional jitter of the optical tweezers. Combining static geometric insensitivity, programmable molecular motion, and partial Raman sideband cooling, we generate two-molecule entanglement with a Bell-state fidelity of
F=0.976−0.011+0.008 in directly laser-cooled molecules. Crucially, the high-fidelity molecular entanglement here is performed without ground-state preparation. Rather than relying on stringent cooling or species-specific trapping conditions, as in prior work, the methods demonstrated here are instead based on dynamic and static geometric control of interacting molecules and are therefore broadly applicable across molecular platforms. These results extend moving optical tweezers beyond assembly and rearrangement, opening routes to robust two-qubit gates, many-body dynamics, and dynamically programmable networks of interaction.
Precision measurements exploit internal molecular structure to search for physics beyond the Standard Model. Reaching the entanglement-enhanced regime requires preparing and preserving correlated molecular states within the same manifold used for sensing. Parity-doublet states are central to proposals for precision measurements with polyatomic molecules because they enable large molecular polarization for enhanced sensitivity, and provide internal state co-magnetometry to suppress systematic errors. Here we report the observation and control of resonant dipolar exchange interactions in a parity-doublet sensing manifold of ultracold polyatomic molecules. Using laser-cooled CaOH molecules in a crossed optical dipole trap, we encode a pseudospin in the
ℓ-type parity-doublet states and observe two complementary signatures of interactions: a density-dependent Ramsey contrast decay and a spin-projection-dependent mean-field precession whose sign reverses with the initialized population imbalance. Both observables are well described by a common discrete truncated Wigner model using independently calibrated experimental parameters. We further Floquet-engineer the interaction anisotropy and observe suppressed many-body dephasing near the SU(2)-symmetric Heisenberg point, identifying a protected regime relevant for spin squeezing and precision measurement with dense molecular ensembles. Our results establish parity doublets as a coherent, interacting, and programmable molecular degree of freedom, connecting the polyatomic precision-measurement platform to dipolar many-body physics and opening a route to entanglement-enhanced tests of fundamental physics.
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.