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We bring out novel dielectric behavior of a spin-chain compound, Ca 3 Co 2 O 6 , undergoing Néel order at ( T N   = ) 24 K. It is found that the virgin curve in the plot of isothermal dielectric constant (ε') versus magnetic-field lies outside the ‘butterfly-shaped’ envelope curve well below  T N   (e.g., 2.6 K), with a signature of a partial arrest of the high-field magnetoelectric (ME) phase in zero-field after travelling through magnetic-field-induced magnetic transitions. This behavior is in contrast to that observed in the isothermal magnetization data. Thus, this work brings out a novel case for ‘phase-coexistence phenomenon’ due to ME coupling. Another strange finding is that there is a weak, but a broad, peak in ε' around 85–115 K well above  T N  , attributable to incipient spin-chain magnetic ordering. This finding should inspire further work to study ME coupling on artificial assemblies of magnetic chains, also keeping in mind miniaturization required for possible applications.

Novel dielectric anomalies due to spin-chains above and below Néel temperature in Ca3Co2O6