Nuclear magnetization distribution effect in molecules: Ra$^+$ and RaF hyperfine structure

TL;DR

This paper develops a method to accurately predict the hyperfine structure of molecules like RaF by accounting for the finite magnetization distribution of the nucleus, using a parameter derived from experimental and theoretical data.

Contribution

It introduces a model-independent approach to include the Bohr-Weisskopf effect in hyperfine structure calculations for atoms and molecules.

Findings

The finite nuclear magnetization distribution contributes up to 4% to the hyperfine structure of RaF.

The method allows separating nuclear and electronic effects in hyperfine calculations.

Application to Ra$^+$ and RaF demonstrates improved prediction accuracy.

Abstract

Recently the first laser spectroscopy measurement of the radioactive RaF molecule has been reported by Ruiz \textit{et al.} [Nature \textbf{581}, 396 (2020)]. This and similar molecules are considered to search for the New Physics effects. The radium nucleus is of interest as it is octupole-deformed and has close levels of opposite parity. The preparation of such experiments can be simplified if there are reliable theoretical predictions. It is shown that the accurate prediction of the hyperfine structure of the RaF molecule requires to take into account the finite magnetization distribution inside the radium nucleus. For atoms, this effect is known as the Bohr-Weisskopf (BW) effect. Its magnitude depends on the model of the nuclear magnetization distribution which is usually not well known. We show that it is possible to express the nuclear magnetization distribution contribution to the hyperfine structure constant in terms of one magnetization distribution dependent parameter: BW matrix element for $1s$-state of the corresponding hydrogen-like ion. This parameter can be extracted from the accurate experimental and theoretical electronic structure data for an ion, atom, or molecule without the explicit treatment of any nuclear magnetization distribution model. This approach can be applied to predict the hyperfine structure of atoms and \textit{molecules} and allows one to separate the nuclear and electronic correlation problems. It is employed to calculate the finite nuclear magnetization distribution contribution to the hyperfine structure of the $^{225}$Ra$^+$ cation and $^{225}$RaF molecule. For the ground state of the $^{225}$RaF molecule, this contribution achieves 4\%.