We present careful experiments on the spin order and multiferroicity of Mn-deficient Ca3CoMn1-xO6 with respect to the Co/Mn compensated Ca3Co1+yMn1-yO6. It is revealed that a slight destruction of the Co/Mn ionic order does not damage but significantly enhances the ferroelectricity in terms of the transition point and polarization magnitude, due to the Mn-deficiency enhanced degree of Co/Mn spin ordering in comparison with Ca3Co1+yMn1-yO6. The delicate competition between the ionic (charge) order and spin frustration is the core physics for improving the ferroelectric performance. (C) 2012 American Institute of Physics. [doi:10.1063/1.3670967]
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