Theoretical investigation on multiple bonds in terminal actinide nitride complexes

Area of Science:

• Inorganic Chemistry
• Computational Chemistry
• Quantum Chemistry

Background:

• Actinide (An) compounds exhibit unique bonding due to relativistic effects.
• Understanding An-N multiple bonds is crucial for novel material design.
• Scalar relativistic DFT provides insights into electronic structures.

Purpose of the Study:

• Investigate the geometric and electronic structures of L-An-N compounds.
• Analyze the bonding nature of actinide-nitrogen multiple bonds.
• Elucidate trends in bonding across the actinide series.

Main Methods:

• Scalar relativistic density functional theory (DFT) calculations.
• Natural Bond Orbital (NBO) analysis.
• Topological analysis of electron density.

Main Results:

• Actinide contraction leads to decreasing An-N bond lengths.
• Mayer bond order and bond strength decrease from Pa to Pu.
• The 6d orbital contributes more to An-N covalency than the 5f orbital.

Conclusions:

• The study clarifies the bonding characteristics of An-N multiple bonds.
• Trends in electronic structure and bonding across the actinide series are elucidated.
• Findings aid in the design of new actinide-nitrogen compounds.