Precision frequency-comb terahertz spectroscopy on pure quantum states of a single molecular ion

Abstract

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 generally applicable 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 non-destructively, leaving the molecule ready for further manipulation. We resolve rotational transitions to 11 significant digits and derive the rotational constant of CaH+ to be B_R = 142501777.9(1.7) kHz. Our approach suits a wide range of molecular ions, including polyatomics and species relevant for tests of fundamental physics, chemistry, and astrophysics.

arXiv comment25 pages, 4 figures, 6 tables

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Cited by in corpus (46)

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• Spin qudit tomography and state reconstruction error
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• Large Vibrationally Induced Parity Violation Effects in CHDBrI${}^{+}$ $-$ A Promising Candidate for Future Experiments
• Strategies for implementing quantum error correction in molecular rotation
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• Quantum control of a single ${\mathrm{H}}_2^{+}$ molecular ion
• Photodissociation spectra of single trapped CaOH+ molecular ions
• Dynamics of translational and rotational thermalization of AlF molecules via collisions with cryogenic helium
• Unresolved sideband photon recoil spectroscopy of molecular ions
• Probing rotational decoherence with a trapped-ion planar rotor
• Protocol for Optically Pumping AlH${}^{+}$ to a Pure Quantum State
• Deterministic preparation of a dual-species two-ion crystal
• Adiabatically controlled motional states of a ground-state cooled CaO${}^{+}$ and Ca${}^{+}$ trapped ion chain
• Precise Determination of Excited State Rotational Constants and Black-Body Thermometry in Coulomb Crystals of Ca${}^{+}$ and CaH${}^{+}$
• Blackbody Radiation Noise Broadening of Quantum Systems
• Ro-vibrational spin-averaged transitions in the hydrogen molecular ions
• Spontaneous Raman scattering out of a metastable atomic qubit
• Molecular Quantum Control Algorithm Design by Reinforcement Learning
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• Electric field dissociation of weakly bound molecular ions
• Radioactive Molecules as Laboratories of Fundamental Physics
• Pump-Threshold-Free Frequency Comb via Cavity Floquet Engineering
• Charge Exchange Dynamics in Cold Collisions of ${}^{40}$CaH${}^{+}$ and ${}^{39}$K