Abstract
Polyatomic molecules have rich structural features that make them uniquely suited to applications in quantum information science1,2,3, quantum simulation4,5,6, ultracold chemistry7 and searches for physics beyond the standard model8,9,10. However, a key challenge is fully controlling both the internal quantum state and the motional degrees of freedom of the molecules. Here we demonstrate the creation of an optical tweezer array of individual polyatomic molecules, CaOH, with quantum control of their internal quantum state. The complex quantum structure of CaOH results in a non-trivial dependence of the molecules’ behaviour on the tweezer light wavelength. We control this interaction and directly and non-destructively image individual molecules in the tweezer array with a fidelity greater than 90%. The molecules are manipulated at the single internal quantum state level, thus demonstrating coherent state control in a tweezer array. The platform demonstrated here will enable a variety of experiments using individual polyatomic molecules with arbitrary spatial arrangement.
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Data availability
The data that support the findings of this study are available from the corresponding author on reasonable request. Source data are provided with this paper.
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Acknowledgements
We thank L. Cheng for providing dynamic polarizability calculations. This work was supported by the AFOSR, NSF, and ARO. Support is also acknowledged from the U.S. Department of Energy, Office of Science, National Quantum Information Science Research Centers, Quantum Systems Accelerator. P.R. acknowledges support from the NSF GRFP, and G.K.L. and L.A. acknowledge support from the HQI.
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N.B.V., P.R., C.H., G.K.L. and L.A. performed the experiment and analysed the data. J.M.D. directed the study. All authors discussed the results and contributed to the manuscript.
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Extended data figures and tables
Extended Data Fig. 1 Imaging photon budget vs. tweezer wavelength.
Calculated (curves) and measured (points) number of imaging photons that can be scattered during molecule imaging in the tweezer array, as a function of the trapping wavelength. Calculations include the effect of vacuum loss, loss to vibrational dark states, and trap-wavelength-dependent excitation to lossy excited electronic levels. The solid blue curve accounts for excitation only to those states observed using AC Stark shift data, while the black, dashed curve additionally includes \({\widetilde{A}}^{2}{\Pi }_{1/2}(000)\leftrightarrow {\widetilde{D}}^{2}{\Sigma }^{+}(010)\) excitation predicted at 793.6 nm.
Extended Data Fig. 2 Determination of tweezer imaging fidelities.
a, Signal (orange) and background (purple) histogram data, hexp(n) and h0(n), for 7 ms tweezer images. The average tweezer loading probability in the signal histogram is p = 0.34. b, Misidentification error rates ϵ01(θ) and ϵ10(θ) for 7 ms tweezer images, inferred from the experimental data as described in the text. c, Imaging fidelities f(p) for several average tweezer loading probabilities p, as described in the text.
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Vilas, N.B., Robichaud, P., Hallas, C. et al. An optical tweezer array of ultracold polyatomic molecules. Nature 628, 282–286 (2024). https://doi.org/10.1038/s41586-024-07199-1
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DOI: https://doi.org/10.1038/s41586-024-07199-1
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