Momentum-resolved observations of the phonon instability driving geometric improper ferroelectricity in yttrium manganite

Dipanshu Bansal (), Jennifer L. Niedziela, Ryan Sinclair, V. Ovidiu Garlea, Douglas L. Abernathy, Songxue Chi, Yang Ren, Haidong Zhou and Olivier Delaire ()
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Dipanshu Bansal: Duke University
Jennifer L. Niedziela: Duke University
Ryan Sinclair: University of Tennessee
V. Ovidiu Garlea: Oak Ridge National Laboratory
Douglas L. Abernathy: Oak Ridge National Laboratory
Songxue Chi: Oak Ridge National Laboratory
Yang Ren: Argonne National Laboratory
Haidong Zhou: University of Tennessee
Olivier Delaire: Duke University

Nature Communications, 2018, vol. 9, issue 1, 1-9

Abstract: Abstract Magnetoelectrics offer tantalizing opportunities for devices coupling ferroelectricity and magnetism but remain difficult to realize. Breakthrough strategies could circumvent the mutually exclusive origins of magnetism and ferroelectricity by exploiting the interaction of multiple phonon modes in geometric improper and hybrid improper ferroelectrics. Yet, the proposed instability of a zone-boundary phonon mode, driving the emergence of ferroelectricity via coupling to a polar mode, remains to be directly observed. Here, we provide previously missing evidence for this scenario in the archetypal improper ferroelectric, yttrium manganite, through comprehensive scattering measurements of the atomic structure and phonons, supported with first-principles simulations. Our experiments and theoretical modeling resolve the origin of the unusual temperature dependence of the polarization and rule out a reported double-step ferroelectric transition. These results emphasize the critical role of phonon anharmonicity in rationalizing lattice instabilities in improper ferroelectrics and show that including these effects in simulations could facilitate the design of magnetoelectrics.

Date: 2018
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DOI: 10.1038/s41467-017-02309-2

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