Spectroscopic Detection and Characterization of Cyanooxomethylium, NCCO

Cyanooxomethylium, NCCO⁺, a fundamental linear acylium ion, has been observed spectroscopically for the first time using action spectroscopy in ion trap apparatuses. A first low-resolution infrared spectrum was obtained between 500 to 1400 cm^-1 and 2000 to 2500 cm^-1 using the Free Electron Laser for Infrared eXperiments (FELIX) and the FELion apparatus, employing infrared predissociation of the weakly bound NCCO⁺-Ne complex. Subsequently, high-resolution studies of the bare ion were performed with the COLtrap II setup, one targeted at the CN-stretching mode ν₂ around 2150 cm^-1 using leak-out spectroscopy and one at the pure rotational spectrum employing a leak-out infrared/millimeter-wave double resonance approach covering transition frequencies as high as 246 GHz. Spectroscopic detection and analysis were guided by high-level quantum-chemical calculations performed at the CCSD(T) level of theory. The collected data permit accurate frequency predictions to support future astronomical searches with sensitive radio telescopes.