Accurate \textit{ab initio} calculations of RaF electronic structure indicate the need for more laser-spectroscopical measurements

Abstract

Recently a breakthrough has been achieved in laser-spectroscopic studies of short-lived radioactive compounds with the first measurements of the radium monofluoride molecule (RaF) UV/vis spectra. We report results from high accuracy \emph{ab initio} calculations of the RaF electronic structure for ground and low-lying excited electronic states. Two different methods agree excellently with experimental excitation energies from the electronic ground state to the ${}^2{\Pi }_{1/2}$ and ${}^2{\Pi }_{3/2}$ states, but lead consistently and unambiguously to deviations from experimental-based adiabatic transition energy estimates for the ${}^2{\Sigma }_{1/2}$ excited electronic state and show that more measurements are needed to clarify spectroscopic assignment of the ${}^2\Delta$ states.

7 pages, 1 figure, 1 table

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Cited by in corpus (12)

• 4-component relativistic Hamiltonian with effective QED potentials for molecular calculations
• Generalized relativistic small-core pseudopotentials accounting for quantum electrodynamic effects: construction and pilot applications
• Laser-coolable AcOH${}^{+}$ ion for $\mathcal{C}\mathcal{P}$-violation searches
• Pinning down electron correlations in RaF via spectroscopy of excited states and high-accuracy relativistic quantum chemistry
• Intensity-borrowing mechanisms pertinent to laser cooling of linear polyatomic molecules
• Theoretical molecular spectroscopy of actinide compounds: The ThO molecule
• Relativistic Exact Two-Component Coupled-Cluster Study of Molecular Sensitivity Factors for Nuclear Schiff Moments
• Ab initio study of electronic states and radiative properties of the AcF molecule
• Observation of the distribution of nuclear magnetization in a molecule
• Radium-containing molecular cations amenable for laser cooling
• Finite-order method to calculate approximate density matrices in the Fock-space multireference coupled cluster theory
• Production and spectroscopy of cold radioactive molecules