We image simultaneously the geometric, electronic and magnetic structure of a buckled iron bilayer film that exhibits chiral magnetic order. We achieve this by combining spin-polarized scanning tunneling microscopy and magnetic exchange force microscopy (SPEX), to independently characterize the geometric as well as the electronic and magnetic structure of non-flat surfaces.This new SPEX imaging technique reveals the geometric height corrugation of the reconstruction lines resulting from strong strain relaxation in the bilayer, enabling the decomposition of the realspace from the eletronic structure at the atomic level, and the correlation with the resultant spin spiral ground state. By additionally utilizing adatom manipulation, we reveal the chiral magnetic ground state of portions of the unit cell that were not previously imaged with SP-STM alone. Using density functional theory (DFT), we investigate the structural and electronic properties of the reconstructed bilayer and identify the favorable stoichiometry regime in agreement with our experimental result.

We investigate the interplay between the structural reconstruction and the magnetic properties of Fe doublelayers on Ir (111)-substrate using first-principles calculations based on density functional theory and mapping of the total energies on an atomistic spin model. We show that, if a second Fe monolayer is deposited on Fe/Ir (111), the stacking may change from hexagonal close-packed to bcc (110)-like accompanied by a reduction of symmetry from trigonal to centered rectangular. Although the bcc-like surface has a lower coordination, we find that this is the structural ground state. This reconstruction has a major impact on the magnetic structure. We investigate in detail the changes in the magnetic exchange interaction, the magnetocrystalline anisotropy, and the Dzyaloshinskii Moriya interaction depending on the stacking sequence of the Fe double-layer. Based on our findings, we suggest a new technique to engineer Dzyaloshinskii Moriya interactions in multilayer systems employing symmetry considerations. The resulting anisotropic Dzyaloshinskii-Moriya interactions may stabilize higher-order skyrmions or antiskyrmions.