The local distortion indicated by the split of the Cu/Sn-Mn bonds for the negative thermal expansion (NTE) materials Cu1−xSnxNMn3 (x = 0.1 and 0.5) was observed using neutron pair distribution function. The distribution of Cu/Sn-Mn bonds upon Sn doping is suggested to be attributable to the fluctuation in the hybridization of Mn d with Sn p orbitals. Accordingly, the antiferromagnetic (AFM) coupling mediated by the p-d hybridization fluctuates in strength. Consequently, the AFM transition closely coupled with the volume change is broadened, leading to the NTE.
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