Compensated Ferrimagnets with Colossal Spin Splitting in Organic Compounds

The study of the magnetic order has recently been invigorated by the discovery of exotic collinear antiferromagnets with time-reversal symmetry breaking. Examples include altermagnets and compensated ferrimagnets, which show spin splittings of the electronic band structures even at zero net magnetization, leading to several unique transport phenomena, notably spin-current generation. Altermagnets demonstrate anisotropic spin splitting, such as $d$-wave, in momentum space, whereas compensated ferrimagnets exhibit isotropic spin splitting. However, methods to realize compensated ferrimagnets are limited. Here, we demonstrate a method to realize a fully compensated ferrimagnet with isotropic spin splitting utilizing the dimer structures inherent in organic compounds. Moreover, based on ab initio calculations, we find that this compensated ferrimagnet can be realized in the recently discovered organic compound ${\left(\mathrm{EDO}\text{−}\mathrm{TTF}\text{−}I\right)}_2{\mathrm{ClO}}_4$. Our findings provide an unprecedented strategy for using the dimer degrees of freedom in organic compounds to realize fully compensated ferrimagnets with colossal spin splitting.