Singlet ground state actinide chemistry with geminals

Area of Science:

• Computational chemistry
• Quantum chemistry
• Actinide chemistry

Background:

• Accurate modeling of heavy-element compounds is computationally demanding.
• Standard quantum chemistry methods face challenges with actinide electronic structures.

Purpose of the Study:

• To apply the novel vOO-AP1roG method to singlet-state actinide chemistry.
• To assess the accuracy and reliability of the AP1roG ansatz for actinide compounds.
• To compare vOO-AP1roG with established quantum chemistry approaches.

Main Methods:

• Application of the variationally orbital optimized antisymmetric product of 1-reference orbital geminals (vOO-AP1roG) method.
• Modeling of ground-state electronic structure for small actinide compounds.
• Comparison with standard quantum chemistry techniques.

Main Results:

• vOO-AP1roG accurately describes the electronic structure of heavy-element compounds.
• Calculated spectroscopic constants (bond lengths, vibrational frequencies) and potential energy curves for UO2(2+) and ThO2 were reliable.
• Energetic stability of ThC2 isomers was accurately predicted.

Conclusions:

• The vOO-AP1roG method provides an accurate and computationally efficient approach for studying actinide chemistry.
• This method offers a reliable alternative for modeling the electronic structure of heavy-element systems.
• The findings pave the way for more accessible studies in actinide research.