Abstract
Magnetism of pure electrons is fundamental for understanding diverse magnetic phenomena in condensed matters but has not been fully investigated in experiments due to the lack of a tractable model system. Such an exotic material necessitates an exclusive magnetic interaction of electrons being devoid of orbital and lattice degrees of freedom. Here, we report the two-dimensional mixed-cation [YGdC]2+∙2e− electride, showing ferrimagnetic nature from the direct exchange interaction of magnetic interstitial electrons in interlayer space. We identify that magnetic interstitial electrons are periodically localized in octahedral and tetrahedral cavities between 2D cationic Y2−xGdx arrays. The mixed configuration of non-magnetic and magnetic cations in cavities induces divergent spin states and interactions of magnetic interstitial electrons, in which their direct exchange interaction overwhelms the interactions with magnetic cations, triggering the ferrimagnetic spin-alignment. This discovery facilitates further exploration of magnetic electrides and nurtures the study of two-dimensional magnetism of layered crystals and electron phases.
Highlights
Understanding the nature of magnetic interaction in the pure electron systems has been of fundamental importance in manybody physics, giving a basic knowledge for the magnetism of condensed matters[1,2,3,4,5,6]
This can allow an exotic magnetism of interstitial electrons in the 2D free space of the electride crystals, substantiating the predicted magnetism of pure electron systems[6,23]
It is noted that the interlayer space occupied by the interstitial anionic electrons (IAEs) is periodically disassembled into three cavities according to their electron density: (1) one six-coordinate octahedral cavity with a high-density IAEs and (2) two fourcoordinate tetrahedral cavities with a low-density IAEs
Summary
Understanding the nature of magnetic interaction in the pure electron systems has been of fundamental importance in manybody physics, giving a basic knowledge for the magnetism of condensed matters[1,2,3,4,5,6]. The magnetic interaction of electrons in real materials has exclusively limited to the orbital electrons[10,11,12,13], not isolated electrons from the electrostatic attraction of the atomic nucleus, provoking the only theoretical perspective for the magnetism of pure electrons In this regard, the electrides, in which anionic electrons are localized at the interstitial space in a crystal lattice, not at the orbitals of constituent elements[14,15,16,17,18], can be considered as a platform to study the inherent magnetism of electrons. Considering that the magnetic IAEs are localized in a 2D potential well of positively charged layers, their spin states can be manipulated to have a direct exchange interaction by enhancing the magnetic instability in the 2D cationic array This can allow an exotic magnetism of interstitial electrons in the 2D free space of the electride crystals, substantiating the predicted magnetism of pure electron systems[6,23]. We design the 2D mixedcation [Y2−xGdxC]2+∙2e− electride, in which an emergent magnetism of interstitial electrons evolves by their direct exchange interaction within 2D space, showing the unprecedented ferrimagnetic spin-alignment
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