First-principles calculations are conducted to compute linear magnetoelectric coupling coefficients in epitaxial (001) ${\mathrm{Sr}}_{0.5}{\mathrm{Ba}}_{0.5}{\mathrm{MnO}}_3$ films. A large enhancement of different linear magnetoelectric elements is found in a strained-induced morphotropic phase boundary region. Such enhancement is demonstrated to originate from the behavior of the dielectric susceptibility, thanks to a simple phenomenological model that is presently shown to be relevant and accurate. This work can thus provide a promising approach towards designing highly desired single-phase multiferroic with a colossal magnetoelectric conversion.

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• Antiferromagnetism
• Dielectric properties
• Epitaxial strain
• Magnetic susceptibility
• Magnetoelectric effect
• Second order phase transitions
• Structural phase transition
• Multiferroics
• Thin films
• Density functional theory
• First-principles calculations