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arXiv:2401.13593 · PRX Quantum

Enhanced Quantum Control of Individual Ultracold Molecules Using Optical Tweezer Arrays

Daniel K. Ruttley, Alexander Guttridge, Tom R. Hepworth, Simon L. Cornish

Published May 13, 2024• 40 citations
arXivHTMLPDF

Abstract

Control over the quantum states of individual molecules is crucial in the quest to harness their rich internal structure and dipolar interactions for applications in quantum science. In this paper, we develop a toolbox of techniques for the control and readout of individually trapped polar molecules in an array of optical tweezers. Starting with arrays of up to eight Rb and eight Cs atoms, we assemble arrays of RbCs molecules in their rovibrational and hyperfine ground state with an overall efficiency of 48(2)%. We demonstrate global microwave control of multiple rotational states of the molecules and use an auxiliary tweezer array to implement site-resolved addressing and state control. We show how the rotational state of the molecule can be mapped onto the position of Rb atoms and use this capability to readout multiple rotational states in a single experimental run. Further, using a scheme for the midsequence detection of molecule formation errors, we perform rearrangement of assembled molecules to prepare small defect-free arrays. Finally, we discuss a feasible route to scaling to larger arrays of molecules. Published by the American Physical Society 2024

DOI
10.1103/prxquantum.5.020333

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Control over the quantum states of individual molecules is crucial in the quest to harness their rich internal structure and dipolar interactions for applications in quantum science. In this paper, we develop a toolbox of techniques for the control and readout of individually trapped polar molecules in an array of optical tweezers. Starting with arrays of up to eight Rb and eight Cs atoms, we assemble arrays of RbCs molecules in their rovibrational and hyperfine ground state with an overall efficiency of 48(2)%. We demonstrate global microwave control of multiple rotational states of the molecules and use an auxiliary tweezer array to implement site-resolved addressing and state control. We show how the rotational state of the molecule can be mapped onto the position of Rb atoms and use this capability to readout multiple rotational states in a single experimental run. Further, using a scheme for the midsequence detection of molecule formation errors, we perform rearrangement of assembled molecules to prepare small defect-free arrays. Finally, we discuss a feasible route to scaling to larger arrays of molecules. Published by the American Physical Society 2024
Polar molecules are a quantum resource with rich internal structure that can be coherently controlled. The structure, however, also makes the state preparation and measurement (SPAM) of molecules challenging. We advance the SPAM of individual molecules assembled from constituent atoms trapped in optical-tweezer arrays. Sites without Na Cs molecules are eliminated using high-fidelity Cs atom detection, increasing the peak molecule filling fraction of the array threefold. We site-selectively initialize the array in a rotational qubit subspace that is insensitive to differential ac Stark shifts from the optical tweezer. Lastly, we detect multiple rotational states per experimental cycle by imaging atoms after sequential state-selective dissociations. These demonstrations extend the SPAM capabilities of molecules for quantum information, simulation, and metrology. Published by the American Physical Society 2024
Abstract Fully internal and motional state controlled and individually manipulable polar molecules are desirable for many quantum science applications leveraging the rich state space and intrinsic interactions of molecules. While prior efforts at assembling molecules from their constituent atoms individually trapped in optical tweezers achieved such a goal for exactly one molecule (Zhang J T et al 2020 Phys. Rev. Lett. 124 253401; Cairncross W B et al 2021 Phys. Rev. Lett. 126 123402; He X et al 2020 Science 370 331–5), here we extend the technique to an array of five molecules, unlocking the ability to study molecular interactions. We detail the technical challenges and solutions inherent in scaling this system up. With parallel preparation and control of multiple molecules in hand, this platform now serves as a starting point to harness the vast resources and long-range dipolar interactions of molecules.
Fully internal and motional state controlled and individually manipulable polar molecules are desirable for many quantum science applications leveraging the rich state space and intrinsic interactions of molecules. While prior efforts at assembling molecules from their constituent atoms individually trapped in optical tweezers achieved such a goal for exactly one molecule, here we extend the technique to an array of five molecules, unlocking the ability to study molecular interactions. We detail the technical challenges and solutions inherent in scaling this system up. With parallel preparation and control of multiple molecules in hand, this platform now serves as a starting point to harness the vast resources and long-range dipolar interactions of molecules.
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.
Optical tweezer arrays trapping ultracold atoms and molecules are a versatile quantum science platform with broad impact in quantum simulation, quantum computation, and quantum metrology. The polarization dependence of anisotropic vector and tensor light shifts offers a degree of freedom for precise quantum state engineering of trapped particles. Similarly, state-selective operations depend on the polarization of the addressing light through the atom--light coupling strength. Yet, methods for controlling the polarization of individual tweezers or local addressing beams remain an experimental challenge. Here, we demonstrate independent, site-resolved linear polarization rotation across an optical tweezer array by exploiting the local birefringence tunability of a spatial light modulator. Applying this capability to an array of 88Sr^{88}\rm{Sr}88Sr atoms, we homogenize differential light shifts imparted by the 813-nm tweezers to the narrow 1S0↔3P1{^1{\rm S}_0}\leftrightarrow{^3{\rm P}_1}1S0​↔3P1​ transition, enabling sideband cooling under a magic-angle condition. Furthermore, we show dynamic transport of trapped atoms across distinct polarization zones with high survival and preserved coherence. Finally, we characterize tweezer polarization noise and demonstrate closed-loop stabilization referenced to the atomic transition frequency, reaching mrad-level stability. Our work establishes a technique for manipulating polarization-sensitive atomic and molecular transitions in tweezer architectures, with immediate applications to optical tweezer clocks and multi-zone quantum processors.