Large-scale density functional theory simulation of inorganic nanotubes: A case study on Imogolite nanotubes

Abstract

The high experimental control over inorganic Imogolite-like open-ended nanotubes (Imo-NTs) composition, dimensions and monodispersity together with the potentially huge range of tuneable properties that can be introduced by chemical functionalisation and doping make Imo-NTs appealing substrates for nanotechnology, as artificial ion-channels and in chemical separation. Investigation of Imo-NTs electronic and spectroscopic properties has so far been hampered by the large size of the systems repeat unit (+300atoms),whichpose severe challenges andaccuracy-viability compromises for standard plane-wave (fixed atomic basis set) density functional theory (DFT) simulations. These challenges can, however, be met by linear-scaling DFT (LS-DFT) approaches based on in situ optimisation of minimal basis sets. Here, we illustrate the applicability of LS-DFT to Imo-NTs by providing structural and electronic characterisation of periodic and finite models of aluminosilicate (AlSi) and methylated-AlSi Imo-NTs. It is shown that adoption of moderate kinetic energy cutoff (1000 eV) and basis set truncation radius (8Bohr) leads to optimal accuracy-viability compromised for geometrical optimisation of Imo-NTs. These results should be useful for future LS-DFT investigation of Imo-NTs and other AlSi-based functional materials.