  The interfaces between organic molecules and metal surfaces with layered
antiferromagnetic order have gained increasing interests in the field of
antiferromagnetic spintronics. The C60 layered AFM spinterfaces have been
studied for C60 bonded only to the outermost ferromagnetic layer. Using density
functional theory calculations, here we demonstrate that C60 adsorption can
reconstruct the layered AFM Cr(001) surface so that C60 bonds to the top two Cr
layers with opposite spin direction. Surface reconstruction drastically changes
C60 s spintronic properties 1 the spin-split p-d hybridization involve
multi-orbitals of C60 and metal double layers, 2 the subsurface layer dominates
the C60 spin properties, and 3) reconstruction induces a large magnetic moment
in C60 of 0.58 B, which is a synergetic effect of the top two layers as a
result of a magnetic direct-exchange interaction. Understanding these complex
spinterfaces phenomena is a crucial step for their device applications. The
surface reconstruction can be realized by annealing at above room temperature
in experiments.
