Atomically Modulating Competing Exchange Interactions in Centrosymmetric Skyrmion Hosts GdRu2X2 (X = Si, Ge)

Abstract: Magnetic skyrmions are topologically protected spin states enabling high-density, low-power spin electronics. Despite growing efforts to find new skyrmion host systems, the microscopic mechanisms leading to skyrmion phase transitions at specific temperatures and magnetic fields remain elusive. Here, we systematically study the isostructural centrosymmetric magnets- GdRu2X2 (X = Si and Ge), and the role of X-p orbitals in modifying magnetic exchange interactions. GdRu2Ge2 single crystals, synthesized by arc melting, exhibit two high-entropy pockets associated with skyrmion phases at 0.9 T < H < 1.2 T and 1.3 T < H < 1.7 T, 2 K < T < 30 K-more accessible condition at lower fields and higher temperatures than that in the Si counterpart. Entropy estimations from heat capacity measurements align with magnetization data, and transport studies confirm a topological Hall effect, highlighting the system's nontrivial spin textures and Berry curvature. Compared to GdRu2Si2, electronic structure and exchange interaction evaluations reveal the more extended Ge-4p orbitals enhance competing exchange interactions in GdRu2Ge2, thereby manifesting the rich skyrmion behavior. This work demonstrates how modifying exchange interactions at the atomic level enables the tunability of topologically nontrivial electronic states while advancing our understanding of skyrmion formation mechanisms for future spintronics.