In silico design criteria for high blocking barrier uranium (iii) SIMs

Abstract

A combination of DFT and ab initio CASSCF/PT2 calculations on U(III) fictitious models and numerous reported X-ray structures unveils several geometries from coordination number 1 to 12 that can be targeted to design potential U(III) SIMs with attractive barrier heights. Among the geometries studied, the T-shaped and capped pentagonal antiprism geometries yield values exceeding 1500 cm⁻¹ – a value that is elusive for any uranium SIMs.