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The paper presents the first observation and coherent manipulation of electric-quadrupole rotational-vibrational transitions in single trapped nitrogen molecular ions (N$_2^+$). They used a quantum-logic-spectroscopy protocol to identify individual hyperfine-Zeeman-rotational components of the fundamental vibrational transition. This allowed for coherent population transfer between energy levels within the molecule.
Quantum computers and molecular clocks just got a boost: researchers have achieved coherent control of forbidden vibrational transitions in single nitrogen molecular ions.
Electric-dipole forbidden spectroscopic transitions in atoms form the basis of many advanced implementations of quantum computers, atomic clocks and quantum sensors. Coherently addressing such transitions in molecules which are among the most ubiquitous and versatile quantum objects has remained a long-standing challenge owing to their complex energy-level structure. Here, we report the search, observation and coherent manipulation of electric-quadrupole rotational-vibrational transitions in single trapped molecules using a quantum-logic-spectroscopy protocol. We identified individual hyperfine-Zeeman-rotational components of the fundamental vibrational transition of the nitrogen molecular ion, N$_2^+$, and performed coherent population transfer between energy levels. Our work opens up new perspectives for precision molecular spectroscopy, for high-fidelity qubits encoded in the rotational-vibrational motion of molecules, for precise infrared molecular clocks and for searches for new physics