Complex magnetic behavior in RuO2 thin films driven by strain and substrate effects

Ruthenium dioxide (RuO2) has been proposed as a prototypical metallic d-wave altermagnet, a Néel-ordered compensated antiferromagnetic state exhibiting nonrelativistic momentum-dependent spin splitting; yet, its magnetic ground state remains controversial both theoretically and experimentally. Using comprehensive first-principles calculations, we investigate RuO2 thin films with (110), (100), and (001) orientations, both (un)strained freestanding and supported on a TiO2 substrate. We show that emergent magnetic moments in RuO2 thin films are highly fragile, strongly influenced by strain, surface orientation, and atomic relaxation, while also being highly sensitive to the choice of the Brillouin-zone integration scheme. We find that none of the thin film structures considered can stabilize a compensated antiferromagnetic order; therefore, an altermagnetic ground state cannot be realized. Instead, substrate-supported RuO2 films on TiO2 exhibit pronounced layer- and site-dependent magnetic moment variations and incomplete compensation between the two antiferromagnetically coupled Ru moments, yielding a ferrimagnetic-like behavior. On the other hand, freestanding RuO2 films display complex magnetic structures depending on their orientation and applied strain, with distinct behavior at the surfaces and in the inner layers. Our results reconcile conflicting theoretical and experimental reports and underscore the sensitivity of RuO2 magnetism to structural and methodological details. Ruthenium dioxide is considered a candidate for metallic d-wave altermagnetism, but its magnetic ground state remains debated. Here, the authors use first-principles calculations to reveal that RuO2 thin films cannot stabilize a compensated antiferromagnetic order, instead exhibiting ferrimagnetic-like behavior influenced by strain, orientation, and substrate effects, clarifying previous discrepancies.