Dipole allowed transitions in GdF: A four-component relativistic general open-shell configuration interaction study

Area of Science:

• Computational Chemistry
• Molecular Spectroscopy
• Relativistic Quantum Chemistry

Background:

• Gadolinium monofluoride (GdF) exhibits complex electronic spectra due to relativistic effects and open-shell electronic configurations.
• Accurate theoretical modeling is crucial for understanding GdF's electronic structure and spectral properties.

Purpose of the Study:

• To perform a four-component relativistic study of electronic transitions in GdF.
• To investigate and refine the electronic spectra of GdF, particularly excited states below 3.0 eV.
• To analyze transitions between excited states and propose a molecular rearrangement.

Main Methods:

• General open-shell configuration interaction (CI) method with active electrons distributed among molecular spinors (Gd 4f, 5d, 6s).
• Valence full-CI-like approach to account for near-degeneracy effects.
• Calculation of transition dipole moments and probabilities.

Main Results:

• Identified candidates for observable electronic transitions based on transition dipole moments.
• Refined the spectra of excited states below 3.0 eV using calculated transition probabilities.
• Newly analyzed transitions between excited states, leading to a proposed rearrangement.

Conclusions:

• The relativistic computational approach provides valuable insights into GdF's electronic transitions.
• The study complements previous experimental and theoretical work on GdF.
• A new analysis of excited state transitions and a proposed molecular rearrangement are presented.