Ferroelectricity with Asymmetric Hysteresis in Metallic LiOsO3 Ultrathin Films

TL;DR

This study demonstrates that ultrathin LiOsO3 films can exhibit switchable ferroelectricity with asymmetric hysteresis, challenging the belief that ferroelectric metals cannot have switchable polar states.

Contribution

The paper reveals that a two-unit-cell LiOsO3 film can have a switchable out-of-plane polarization and introduces an extension of Born effective charge to metallic systems.

Findings

Ultrathin LiOsO3 films show switchable out-of-plane polarization.

Hysteresis loop is asymmetric due to surface ion displacement.

Extension of Born effective charge concept to metals.

Abstract

Bulk LiOsO3 was experimentally identified as a "ferroelectric" metal where polar distortions coexist with metallicity [Shi et al., Nature Materials 12, 1024 (2013)]. It is generally believed that polar displacements in a "ferroelectric" metal cannot be switched by an external electric field. Here, via comprehensive density functional theory calculations, we demonstrate that a two-unit-cell-thick LiOsO3 thin film exhibits a ferroelectric ground state having an out-of-plane electric dipole moment that can be switched by an external electric field. Moreover, its dipole moment-versus-electric-field hysteresis loop is asymmetric because only surface Li ions'displacements are reversed by external electric field whereas the field-induced force on inner Li atoms are nearly fully screened by itinerant electrons. As a relevant by-product of our study, we also extend the concept of "Born effective charge" to finite metallic systems, and show its usefulness to rationalize the observed effects.