Abstract

Quantum computers (QC) which require data to be encoded into qubits ( Ψ=𝛼∣∣0⟩+𝛽∣∣1⟩ ) as opposed to bits (0 or 1) now holds a revolutionary promise to increase storage density, processing speed, and computational efficiency to meet up with future computational demands. However, the development of quantum computers at the moment is limited to extremely low temperatures where existing materials can show such quantum phenomena as qubits. There is the need, therefore, to find the best way to extend this behaviour to temperatures for practical applications. Of prime candidate in the development of quantum computers are single-molecule magnets (SMMs). In the present study, multi-reference ab initio computational methods like the complete active space self-consistence field (CASSCF) was used to model, elucidate and parametrise factors necessary to enhance SMM behaviour in lanthanide-based compounds. The effect of aromatic substituents and chelation on f-orbital splitting as well as the spin transitions were rationalised and by extension comment on their implication to the realisation of single-molecule magnets (SMMs) in materials.