4.8 Article

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

Journal

SCIENCE
Volume 367, Issue 6485, Pages 1458-+

Publisher

AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/science.aba3628

Keywords

-

Funding

  1. U.S. Army Research Office [W911NF-19-1-0172]
  2. National Research Council postdoctoral fellowship
  3. National Key R&D Program of China [2018YFA0306600]
  4. National Natural Science Foundation of China [11974330]
  5. Anhui Initiative in Quantum Information Technologies [AHY050000]
  6. Alexander von Humboldt foundation
  7. state of Baden-Wurttemberg through bwHPC (bwUnicluster) [RV bw17D01]
  8. state of Baden-Wurttemberg through bwHPC (JUSTUS) [RV bw17D01]

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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 (CaH+)-Ca-40 to be B-R = 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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