Supporting Information for Relativistic Density Functional Theory of Actinide Coordination and Redox Chemistry in Molten Fluoride Salts

Data and analysis scripts supporting Relativistic Density Functional Theory of Actinide Coordination and Redox Chemistry in Molten Fluoride Salts (G. Bogolyubov). Relativistic DFT study of Th(IV), U(IV) and U(III) fluoride complexes in fluoride carrier salts, treated both as bare ions and microsolvated in explicit first and second LiF shells, together with adiabatic reduction energies and fluoride-exchange barriers. Every table and figure in the paper and its Supporting Information is generated from the files in this deposit by the scripts included. Contents - structures.zip: Cartesian coordinates for 43 optimized structures (16 bare complexes, 15 microsolvated at +4 LiF, 12 at +8 LiF) in `.xyz` format, with a manifest giving charge, spin multiplicity, level of theory, originating output file and checksum for each.- inputs.zip: ORCA and Gaussian inputs for the bare complexes, microsolvated clusters, relaxed An–F scans, transition states and the four-functional benchmark, plus the actinide basis blocks.- logs.zip: Gaussian outputs for the 13 relaxed scans and 5 transition-state optimizations.- data.zip: harvested results in JSON and CSV: bare-complex energies, geometries, populations and thermochemistry; reduction and reorganization energies; per-point scan profiles; transition-state data.- scripts.zip: extraction, harvesting, input-generation and figure scripts, including the script that regenerates the entire Supporting Information from the harvested data.- figures.zip: publication figures with the ChimeraX render script and `.mol2` inputs.- supporting_information.pdf / .zip: Supporting Information and its LaTeX source. Levels of theory Bare complexes: PBE0/ZORA with the all-electron SARC-ZORA actinide basis and def2-QZVP on F and Li. Microsolvated clusters: UB3LYP/SDD geometries and frequencies with PBE0/ZORA property single points. Scans and transition states: UB3LYP/SDD. Bare and solvated geometries are not interchangeable — on common structures UB3LYP/SDD mean An–F distances exceed PBE0/ZORA by 0.01–0.02 Å for Th(IV) and by up to 0.14 Å for U(III). Two conventions are needed to reproduce the tables Several clusters were optimized more than once. Where variants exist, the structure reported in the paper is selected by the precedence order _L2 > _L > _gd_r > _g_r2 > _g_r > _gd > _g At CN 6 with eight LiF units the `_g` variant gives a uranium spin population of 2.385 and the `_L2` variant 2.080. The paper reports 2.080. Separately, a parallel series of constrained optimizations carries the suffix `_c`. These are excluded from every table in the paper and from this deposit. See `README.md` for the full file listing, reproduction instructions, and two known issues in the source JSON.