In rare-earth orthoferrites, strongly correlated order parameters have been thoroughly investigated, which aims to find multiple functionalities such as multiferroic or magnetoelectric properties. We have discovered highly anisotropic and nonlinear magnetodielectric effects from detailed measurements of magnetoelectric properties in single-crystalline orthoferrite, ErFeO3. Isothermal dielectric constant varies in shapes and signs depending on the relative orientations between the external electric and magnetic fields, which may be ascribed to the spin-phonon couplings. In addition, a dielectric constant with both electric and magnetic fields along the c axis exhibits two symmetric sharp anomalies, which are closely relevant to the spin-flop transition, below the ordering temperature of Er3+ spins, TEr = 3.4 K. We speculate that the magnetostriction from the exchange couplings between Er3+ and Fe3+ magnetic moments would be responsible for this relationship between electric and magnetic properties. Our results present significant characteristics of the orthoferrite compounds and offer a crucial guide for exploring suitable materials for magnetoelectric functional applications.
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