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The interfaces between organic molecules and metal surfaces with layeredantiferromagnetic order have gained increasing interests in the field ofantiferromagnetic spintronics. The C60 layered AFM spinterfaces have beenstudied for C60 bonded only to the outermost ferromagnetic layer. Using densityfunctional theory calculations, here we demonstrate that C60 adsorption canreconstruct the layered AFM Cr(001) surface so that C60 bonds to the top two Crlayers with opposite spin direction. Surface reconstruction drastically changesC60 s spintronic properties 1 the spin-split p-d hybridization involvemulti-orbitals of C60 and metal double layers, 2 the subsurface layer dominatesthe C60 spin properties, and 3) reconstruction induces a large magnetic momentin C60 of 0.58 B, which is a synergetic effect of the top two layers as aresult of a magnetic direct-exchange interaction. Understanding these complexspinterfaces phenomena is a crucial step for their device applications. Thesurface reconstruction can be realized by annealing at above room temperaturein experiments.

Fullerene antiferromagnetic reconstructed spinterface subsurface layer dominates multi-orbitals spin-splitting and large magnetic moment in C60