Orbital Coupling and Spin Textures of Fe/Pd Thin Films Grown on Si Substrate with High Magnetic Fields

Abstract The crystallization and magnetic properties strongly depend on the orbital coupling and spin polarization of magnetic materials. Here, the enhancement and freeze of coupling and polarization of atomic orbitals achieved by high magnetic fields are delineated through the first‐principles calculations. Thus a growth method (under high magnetic fields) is proposed to design the crystallization and magnetic structure of the Fe/Pd thin films. The dynamic processes of film growth are revealed based on the observation of transmission electron microscopy. As the magnetic field increased, the Fe film is found to develop from a unique droplet shape to a 2D growth mode, which is caused by the competition between demagnetization energy and interfacial energy. Furthermore, the improvements achieved by high magnetic fields in macroscopic magnetic properties and ordered magnetic domains are demonstrated, confirming the effective regulation of the orbital coupling and spin textures from this designed method. This work provides a new perspective for understanding the interaction between atomic‐orbital and external magnetic fields and offers a strategy for the preparation of high‐performance magnetoelectric and spintronic devices.