Scattering resonances in bimolecular collisions between NO radicals and H2 challenge the theoretical gold standard

Over the last 25 years, the formalism known as coupled-cluster (CC) theory has emerged as the method of choice for the ab initio calculation of intermolecular interaction potentials. The implementation known as CCSD(T) is often referred to as the gold standard in quantum chemistry. It gives excellent agreement with experimental observations for a variety of energy-transfer processes in molecular collisions, and it is used to calibrate density functional theory. Here, we present measurements of low-energy collisions between NO radicals and H 2 molecules with a resolution that challenges the most sophisticated quantum chemistry calculations at the CCSD(T) level. Using hitherto-unexplored anti-seeding techniques to reduce the collision energy in a crossed-beam inelastic-scattering experiment, a resonance structure near 14 cm −1 is clearly resolved in the state-to-state integral cross-section, and a unique resonance fingerprint is observed in the corresponding differential cross-section. This resonance structure discriminates between two NO–H 2 potentials calculated at the CCSD(T) level and pushes the required accuracy beyond the gold standard. Calculations at the theoretical gold standard generally yield accurate results for a variety of energy-transfer processes in molecular collisions. Using anti-seeding methods in a crossed-beam inelastic scattering experiment, a resonance structure is clearly resolved for NO–H 2 collisions, pushing the required accuracy for theoretical potentials beyond the gold standard.