Quantum-logic spectroscopy of forbidden vibrational transitions in single nitrogen molecular ions

Abstract 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 identify individual hyperfine-Zeeman-rotational components of the fundamental vibrational transition of the nitrogen molecular ion, $${{{{{\rm{N}}}}}}_{2}^{+}$$ N 2 + , and perform 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.