Influence of external field direction on polarization rotation in antiferroelectric squaric acid H$_2$C$_4$O$_4$

TL;DR

This study models how the direction of an external electric field influences polarization rotation and phase transitions in antiferroelectric squaric acid crystals, revealing orientation-dependent behaviors and phase diagrams.

Contribution

It provides a detailed theoretical analysis of polarization rotation processes in squaric acid under arbitrary electric field directions, including phase diagrams and proton configurations.

Findings

Two-step polarization reorientation occurs at most field directions.

The intermediate noncollinear phase is absent when the field aligns with the polarization axis.

Phase diagrams are constructed for specific field orientations.

Abstract

Using the previously developed model we explore the processes of polarization rotation in antiferroelectric crystals of squaric acid by the electric fields directed arbitrarily within the $ac$ plane. Except for some particular directions of the field, the two-step polarization reorientation at low temperatures is predicted: first, to the noncollinear phase with perpendicular sublattice polarizations and then to the collinear ferroelectric phase. However, when the field is directed along the axis of spontaneous sublattice polarizations, the intermediate noncollinear phase is absent; when the field is at 45$^\circ$ to this axis, the field for transition to the ferroelectric phase tends to infinity. The ground state proton configurations and the directions of the sublattice polarization vectors are determined for all field orientations. The $T$-$E$ phase diagrams are constructed for the fields directed along the diagonals of the $ac$ plane and for the above discussed particular directions of the field.