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

## TL;DR

High magnetic fields help control the structure and magnetic properties of Fe/Pd thin films, enabling better performance in spintronic devices.

## Contribution

A new method using high magnetic fields to regulate orbital coupling and spin textures during thin film growth is proposed.

## Key findings

- High magnetic fields promote 2D growth of Fe films and improve magnetic domain uniformity.
- Orbital coupling and spin polarization are enhanced under high magnetic fields.
- The method improves macroscopic magnetic properties and enables precise structural control.

## 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.

High magnetic fields (HMFs) regulate orbital coupling and spin polarization in Fe/Pd thin films, promoting crystallization and ordered spin textures. HMF‐assisted growth transitions Fe from amorphous to dense 2D structures, enhancing saturation magnetization and domain uniformity. This strategy advances the design of high‐performance spintronic devices via precise magnetic and structural control.