Data archive for M. Pizzochero, R. Yadav, and O. V. Yazyev, "Magnetic exchange interactions in monolayer CrI3 from many-body wavefunction calculations", 2D Mater. 7, 035005 (2020). DOI: 10.1088/2053-1583/ab7cab URL: https://iopscience.iop.org/article/10.1088/2053-1583/ab7cab/meta The following archive contain two folders with the following content: 1) DFT-Results : CurieTemperatures.data : Curie temperature of monolayer CrI3 for different xc functionals calculated with the formalism of Torelli et al. [Ref. 58] ExchangeCoupling.data : (twice the) Heisenberg exchange coupling of CrI3 for different xc functionals MagneticAnisotropy.dat : magnetic anisotropy of monolayer CrI3 in the ferromagnetic phase for different xc functionals Fig2.agr : XmGrace file for Figure 2 io_dft : This folder contains the VASP input and output files for the calculations of magnetic interactions in monolayer CrI3 by means of several density-functional approximations. For each functional, we have obtained total energies of four different magnetic configurations (subfolders FM-out-of-plane, FM-in-plane, AFM-out-of-plane, AFM-in-plane). 2) QC-Results: single_ion_anisotropy : g_factors_input.dat : QC input file used to obtain the g_factors as well as single ion anisotropy g_factors_out.dat : the corresponding QC output file cas4_loc : input orbitals used in the g_factors_inp.dat obtained and optimized at the CASSCF level of theory MagneticAnisotropy.dat : processed output obtained from these files and reported in 2D Mater. 7, 035005 (2020). magnetic_exchange_couplings : exchange_coupling_input.dat : QC input file used to calculate magnetic exchange couplings exchange_coupling_output.dat : the corresponding QC output cas_loc_orb : input orbitals used in the exchange_coupling_input.dat obtained and optimized at the CASSCF level of theory. ExchangeCoupling.dat : ontains the processed output obtained from these files and reported in 2D Mater. 7, 035005 (2020).