Global Minimum Search and Bonding Analysis of Tl

Area of Science:

• Inorganic Chemistry
• Computational Chemistry
• Quantum Chemistry

Background:

• Carbon and boron hydrides display distinct bonding and reactivity, leading to varied applications.
• Boron hydrides are known for non-classical structures, while other Group 13 hydrides are less understood.
• Thallium (Tl), the heaviest stable Group 13 element, has limited known hydride chemistry.

Purpose of the Study:

• To explore the hydride chemistry of thallium (Tl2Hx and Tl3Hy).
• To investigate bonding patterns, thermodynamic stability, and electron detachment stability.
• To classify the structural characteristics of thallium hydrides.

Main Methods:

• Conformational analysis using the Coalescence Kick global minimum search algorithm.
• Density Functional Theory (DFT) and ab initio quantum chemistry calculations.
• Analysis of bonding patterns using the Atoms in Molecules (AIM) and the Atoms in Molecules Density-based Pair analysis (AdNDP) algorithms.

Main Results:

• Identified numerous non-classical structures for thallium hydrides (Tl2Hx, Tl3Hy).
• All global minimum structures feature at least one multi-center bond.
• Assessed thermodynamic stability and stability toward electron detachment.

Conclusions:

• Thallium hydrides exhibit unique non-classical bonding, distinct from classical two-center-two-electron bonds.
• The findings expand the understanding of Group 13 hydride chemistry.
• This research provides a foundation for exploring the potential applications of thallium hydrides.