Magnetic quasi-atomic electrons driven reversible structural and magnetic transitions between electride and its hydrides.

In electrides, interstitial anionic electrons (IAEs) in the quantized energy levels at cavities of positively charged lattice framework possess their own magnetic moment and interact with each or surrounding cations, behaving as quasi-atoms and inducing diverse magnetism. Here, we report the reversible structural and magnetic transitions by the substitution of the quasi-atomic IAEs in the ferromagnetic two-dimensional [GdC]·2e electride with hydrogens and subsequent dehydrogenation of the canted antiferromagnetic GdCH (y > 2.0). It is demonstrated that structural and magnetic transitions are strongly coupled by the presence or absence of the magnetic quasi-atomic IAEs and non-magnetic hydrogen anions in the interlayer space, which dominate exchange interactions between out-of-plane Gd-Gd atoms. Furthermore, the magnetic quasi-atomic IAEs are inherently conserved by the hydrogen desorption from the P[Formula: see text] 1m structured GdCH, restoring the original ferromagnetic state of the R[Formula: see text]m structured [GdC]·2e electride. This variable density of magnetic quasi-atomic IAEs enables the quantum manipulation of floating electron phases on the electride surface.