Competing structural instabilities in Bi2SiO5

The lattice dynamics of Bi2SiO5 has been studied by x-ray thermal diffuse scattering (TDS), inelastic x-ray scattering (IXS), and density functional theory calculations across the ferroelectric transition at TC=663 K. Rodlike diffuse features are observed along the [100] direction, perpendicular to the direction of the quasi-one-dimensional silicate chains. IXS measurements of the phonon dispersion along the [100] Γ-Y direction related these diffuse features to coupled unstable transverse optic and acoustic branches. A strong temperature-dependent TDS signal was also observed at the Brillouin zone edges, at the Y and S points, indicating a competition between ferroelectric and antiferroelectric distortions. We observed with IXS a substantial but finite phonon softening at the Y point and a minor softening at the S point, that are associated with the displacement of oxygen atoms. The good agreement between the experiment and the theoretical TDS and IXS allows us to provide a quantitative overview of the various lattice dynamical instabilities occurring at TC. The direct evidence for competing ferroelectric and antiferroelectric orders opens the way towards tuning the properties of Bi2SiO5 by application of pressure or electrical field.