Computational Outputs of Geometry Optimisations, Frequency Calculations, Intrinsic Basis Bonding Analysis and Calculations of the Electric Field Gradients

We provide computational outputs for all calculations conducted during this work.
<p>Geometry optimisations were performed in ORCA 6.0.1 at the B3LYP-D3(BJ,abc)/ma-def2-TZVP level of theory. Additionally, geometry optimisations were performed in Gaussian 16 (Rev. C.01), employing B3LYP-D3(BJ), PBE0-D3(BJ), CAM-B3LYP-D3(BJ), LC-ωPBE-D3(BJ), M06-2X, B2PLYP-D3(BJ), DSD-PBEP86-D3(BJ) and MP2 methods, this includes vibrational perturbation theory calculations of second order (VPT2). Here, the def2-TZVP basis set was used.</p>
<p>Electric field gradient calculations were performed in ORCA 6.0.1 using the B3LYP-D3(BJ,abc)/ma-def2-TZVP geometries. Baileys B1LYP/6-311G(df,p) level of theory alongside PBE/def2-SVP were used. Additionally, B3LYP, B2PLYP, BP86, B97, and B97M-V were combined with the x2c-TZVPPall basis set. Relativistic effects were treated with the second order Douglas-Kroll-Hess transformation (DKH2) as well as the exact two-component theory (X2C) implementation, both in combination with the finite nucleus model and picture change effects.
</p>
<p> Finally, an intrinsic Basis Bonding Analysis (IBBA) at the B3LYP-D3(BJ,abc)/cc-pVTZ-DK level of theory was performed in MOLPRO 2024.1, again using the B3LYP-D3(BJ,abc)/ma-def2-TZVP geometries. Relativistic effects were treated with DKH2 and the finite nucleus model.
</p>
<p> The attached .zip file consists of sub-directories for each of the programs used followed by folders named after the type of calculation and/or the level of theory employed. All output formats are in the ASCII format. The nomenclature follows Fig. 1 of the main publication which is also attached (nomenclature.pdf).</p>