Calculations of neon nuclear-spin optical rotation, Verdet and hyperfine constants with configuration-interaction many-body perturbation theory

Abstract

The nuclear-spin optical rotation (NSOR) effect can enable correlated optical-NMR spectroscopy and imaging. The calculation of NSOR constants is very challenging owing to the high sensitivity to various interactions and neon arguably is a relatively simple atom for calculations. While the neon NSOR effect was not observed and characterized, it can be measured similarly to xenon NSOR to provide data for testing theories. One goal of this paper is to give an estimate of the effect for future experiments in neon. We have calculated the neon NSOR constant using relativistic configuration-interaction many-body perturbation (CI-MBPT). In order to evaluate the accuracy of the CI-MBPT, it was tested on neon energies, oscillator strengths, hyperfine constants and Verdet constants to show a good agreement with experiment. However, the NSOR constant calculations turned out to be more sensitive to the basis set choice, correlation corrections and relativistic effects, which were studied using the CI-MBPT framework. Apart from providing data for future neon NSOR experiments, the CI-MBPT results can be useful for comparison with molecular-structure calculations, as we illustrated on the example of Dalton calculations.The neon atom NSOR is similar to the NSOR of fluorine-containing molecules, to which DALTON calculations can be applied, unlike the atomic CI-MBPT method, so the performance of DALTON calculations in neon can be a good testing ground for F-containing molecules as well.