Frequency-comb spectroscopy on pure quantum states of a single molecular ion

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Science  27 Mar 2020:
Vol. 367, Issue 6485, pp. 1458-1461
DOI: 10.1126/science.aba3628

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Precision spectroscopy with single ions

Spectroscopy is a powerful tool that can identify chemical species used in a wide range of settings. Usually, the samples are formed of ensembles, and this can limit the resolution with which the different species can be detected or identified. Chou et al. demonstrate an optical frequency comb technique with a single pair of trapped ions, Ca+ and CaH+, to obtain the rotational spectrum of a single trapped ion, CaH+. With the ions isolated and the ensemble interactions removed, the rotational structure of the trapped molecular ion can then be obtained with high precision. As the trapping and manipulation process is general, this technique could be applied to a number of chemical species for specific purposes.

Science, this issue p. 1458


Spectroscopy is a powerful tool for studying molecules and is commonly performed on large thermal molecular ensembles that are perturbed by motional shifts and interactions with the environment and one another, resulting in convoluted spectra and limited resolution. Here, we use quantum-logic techniques to prepare a trapped molecular ion in a single quantum state, drive terahertz rotational transitions with an optical frequency comb, and read out the final state nondestructively, leaving the molecule ready for further manipulation. We can resolve rotational transitions to 11 significant digits and derive the rotational constant of 40CaH+ to be BR = 142 501 777.9(1.7) kilohertz. Our approach is suited for a wide range of molecular ions, including polyatomics and species relevant for tests of fundamental physics, chemistry, and astrophysics.

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