A Strain-enabled Novel Multiferroic State in Barium Hexaferrite through Suppression of Quantum Paraelectricity

Barium hexaferrite (BaFe₁₂O₁₉) is predicted to harbor a novel multiferroic phase within which frustrated antiferroelectricity and ferrimagnetism coexist. However, experimental studies have shown that in bulk barium hexaferrite, quantum fluctuations instead lead to a quantum paraelectric ground state at low temperature [1-2]. Strain is a popular method for tuning functional properties in epitaxial thin films and has previously been used to coax ferroic electric dipole order, for example in SrTiO₃ [3]. Similarly, recent theoretical exploration has suggested that strain may enhance antiferroelectricity in barium hexaferrite [4]. In this theoretical work, we combine first-principles calculations with quantum Monte Carlo simulations to explore the temperature- and strain-dependent properties of barium hexaferrite. We find good agreement between our model and available bulk experimental data. In the investigation of strained barium hexaferrite, we find that a modest compressive strain of approximately 1% enables the transition to a frustrated antiferroelectric phase with a critical temperature of greater than 10 K. Our results suggest that further investment in epitaxy and development of compressive substrates for hexaferrites may provide a promising route towards room temperature multiferroics.

[1] Shen et al. Phys. Rev. B 90, 180404(R) (2014)

[2] Zhang et al. Phys. Rev. B 101, 104102 (2020)

[3] Haeni et al. Nature 430 758–761 (2004)

[4] Wang et al. Phys. Rev. X 4, 011035 (2014)