Free Molecule Studies by Perturbed γ-γ Angular Correlation: A New Path to Accurate Nuclear Quadrupole Moments

Accurate nuclear quadrupole moment values are essential as benchmarks for nuclear structure models and for the interpretation of experimentally determined nuclear quadrupole interactions in terms of electronic and molecular structure. Here, we present a novel route to such data by combining perturbed gamma-gamma angular correlation measurements on free small linear molecules, realized for the first time within this work, with state-of-the-art ab initio electronic structure calculations of the electric field gradient at the probe site. This approach, also feasible for a series of other cases, is applied to Hg and Cd halides, resulting in Q(Hg-199, 5/2(-)) = +0.674(17) b and Q(Cd-111, 5/2(+)) = +0.664(7) b.

Automated summary

Accurate nuclear quadrupole moment values are crucial for nuclear structure models and interpreting nuclear interactions. A novel approach combining experimental measurements and electronic structure calculations was introduced, successfully applied to Hg and Cd halides, yielding precise results.