Data for: Host preparation alters Cu substitution energetics in C-(A)-S-H

Structures, CP2K inputs and outputs, energy tables and figure source data for the article 'Host preparation alters Cu substitution energetics in C-(A)-S-H'. Library A contains 50 C-(A)-S-H hosts (six silicate topologies; Al-free, Al–OH and Al–Ca chemistries; up to three proton configurations each) optimised at fixed cell, with 199 Cu-for-Ca substitutions. Library B contains the same hosts re-prepared by annealing with MACE-MP-0 (medium) and D3(BJ), quenching and DFT variable-cell relaxation, with 72 Cu relaxations in 18 hosts (71 matched to library A sites), 20 further sites in five hosts and vertical substitution energies for 196 sites in 49 hosts. Also included are three hosts cell-relaxed directly from library A and their Cu cells, constrained relaxations, alternative starting geometries, PBE+U calculations, and the annealing logs, settings and saved frames. All energies were computed with CP2K 2025.1 (PBE-D3(BJ), DZVP-MOLOPT, GTH pseudopotentials, 800/60 Ry, Γ point). The MACE-MP-0 model file is not included; its hash is given in libb/records/model-files.json. Files: the archive is split into 13 ZIP files (Cu_CASH_data_part1.zip to part13.zip) that extract into one folder, Cu_CASH_data; SHA256SUMS in part 1 lists all files. CP2K outputs and other large text files are xz-compressed. Layout: library A in models/, data/, structures/, inputs/ and raw/; library B, V and control calculations in libb/; article tables in tables/ and figures in figures/. Identifiers: F01–F06 are topologies T1–T6; CSH, ALH and ALC are the Al-free, Al–OH and Al–Ca chemistries; K01–K03 are configurations C1–C3; S01–S02 are main-layer and S03–S04 interlayer sites. Atom indices are zero-based. Units: total energies in Ha (columns ending _Ha), energy differences in eV, distances in Å, densities in g cm⁻³, stress in bar. Empty CSV fields are unavailable values, not zeros.