Archive files with calculations supporting the results discussed in N. Bassi, J. Wilhelm, N. Krane, F. Xiang, P. Čmelová, E. Turco, P. Gargiani, C. A. Pignedoli, M. Juríček, R. Fasel, R. Korytár, P. Ruffieux ACS Nano 19, 38, 33868–33878 (2025). DOI: 10.1021/acsnano.5c09052 pdos.tgz contains the pdos calculations done with Quantum ESPRESSO orbitals.tgz contains cube files of the orbitals of the top and fcc configuration for the TbAu2 surface calculations.aiida contains aiida nodes for calculations of the TbAu2 substrate done with CP2K