Interstitial-Electron Altermagnetism in Two Dimensions

Abstract: Altermagnetism has so far been associated with compensated magnetic moments carried by atoms. Here we introduce Stoner instability induced interstitial-electron altermagnetism, a distinct mechanism in which altermagnetic order is carried instead by interstitial anionic electrons in electrides. We show that, owing to the quasi-nucleus-free nature of interstitial electrons, the Stoner instability in electrides hosting two interstitial electrons can naturally stabilize an altermagnetic state rather than the conventional ferromagnetic one. This mechanism leads to a practical design principle for two-dimensional materials, from which we identify monolayers Zr2N and Ti2N as representative candidates. The strong sensitivity of interstitial electrons to cavity size enables efficient strain control of the altermagnetic order and a pronounced piezo-altermagnetic effect. Moreover, we investigate the evolution of the magnetism in Zr2N under ultrafast laser excitation, which exhibits dynamics distinct from those in all previously reported magnetic materials where magnetism is carried by real atoms. Our work not only offers a novel pathway to realize altermagnetism but also reveals an efficient non-magnetic route for its control.