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Using a molecular beam epitaxy technique, we experimentally demonstrate a multiferroic heterostructure consisting of metastable ferromagnetic Co 3 Mn on piezoelectric Pb(Mg 1 / 3 Nb 2 / 3 )O 3 –PbTiO 3 (PMN-PT). Inserting a 2-nm-thick Fe layer between Co 3 Mn and PMN-PT(001) allows the formation of bcc Co 3 Mn layers even at an extremely low growth temperature of ∼ 80 ° C. Upon increasing this temperature to 200 ° C, a bcc Co 3 Mn/Fe/PMN-PT(001) multiferroic heterostructure with a relatively large saturation magnetization of ∼ 1680 kA/m and an atomically flat interface is obtained, resulting in an obvious converse magnetoelectric (CME) effect. The large CME effect originates mainly from the strain-induced modulation of the magnetic anisotropy energy, supported by the first-principles calculations. [ABSTRACT FROM AUTHOR]