This dataset contains raw computational input and output files for first-principles density-functional theory (DFT) calculations on pristine and vanadium-doped layered metal halide perovskites PEA2PbI4 and PEA2PbBr4 (PEA = phenethylammonium). The calculations support the associated manuscript "Magnetic amplification in 2D halide perovskites by spatially controlled doping." The data include FHI-aims geometry relaxation inputs/outputs and electronic-structure calculations used to analyze band structures, total and projected densities of states and Mulliken band-character information.
