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MnCr2O4 that exhibits spin frustration and complex spiral spin order is ofgreat interest from both fundamental as well as application-orientedperspectives. Unlike CoCr2O4 whose ground state presents the coexistence ofcommensurate spiral spin order (CSSO) and ferroelectric order, MnCr2O4 shows nomultiferroicity. One reason is that the spiral spin order is highly sensitiveto the oxygen concentration in MnCr2O4. Here, we have successfully grownhigh-quality single-crystalline MnCr2O4 by the chemical vapor transport method.We observe a new first-order magnetic transition from the incommensurate spiralspin order (ICSSO) at 19.4 K to the CSSO at 17.4 K. This magnetic transition isverified by magnetization, specific heat, and magnetoelectric measurements,which also confirm that the ground state exhibits the coexistence of the CSSOand magnetoelectricity below 17.4 K. Interestingly, the temperature evolutionof Raman spectra between 5.4 and 300 K suggests that the structure remains thesame. We also find that the phase-transition temperature of the CSSO decreasesas applied magnetic field increases up to 45 kOe.

Magnetoelectric and Raman spectroscopic studies of single-crystalline MnCr2O4