Our ab initio calculations show that half-metallicity can be readily achieved in complex transition metal-cyclopentadienyl TM'-TM_nCp_(n+1) sandwich molecular wires (SMWs). The half-metallicity and ferromagnetism/antiferromagnetism of complex SMWs are found to originate from the coupling between d electrons of TM and TM' atoms via the ligands, which determines the filling of the d bands of TMs. A general "competitive charger-transfer" model is proposed to predict the half-metallicity in complex TM'-TM_nCp_(n+1) SMWs. Furthermore, a series of robust half-metallic ferromagnets, as well as a narrow gap antiferromagnet, are identified using ab initio calculations combined with the model analysis. With tunable electronic and magnetic properties, complex SMWs have profound applications in spintronic devices.
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