Suppression of antiferromagnetic order by strain-enhanced frustration in honeycomb cobaltate.

Layered honeycomb cobaltates are predicted as promising for realizing the Kitaev quantum spin liquid, a many-body quantum entangled ground state characterized by fractional excitations. However, they exhibit antiferromagnetic ordering at low temperatures, hindering the expected quantum state. We demonstrate that controlling the trigonal distortion of CoO6 octahedra is crucial to suppress antiferromagnetic order through enhancing frustration in layered honeycomb cobaltates. Using heterostructure engineering on Cu3Co2SbO6 thin films, we adjust the trigonal distortion of CoO6 octahedra and the resulting trigonal crystal field. The original Néel temperature of 16 kelvin in bulk Cu3Co2SbO6 decreases (increases) to 7.8 kelvin (22.7 kelvin) in strained Cu3Co2SbO6 films by decreasing (increasing) the magnitude of the trigonal crystal fields. The first-principles calculation suggests the enhancement of geometrical frustration as the origin of the suppression of antiferromagnetism. This finding supports the potential of layered honeycomb cobaltate heterostructures and strain engineering in realizing extremely elusive quantum phases of matter.

Ultrahigh dielectric permittivity in oxide ceramics by hydrogenation.

Boosting dielectric permittivity representing electrical polarizability of dielectric materials has been considered a keystone for achieving scientific breakthroughs as well as technological advances in various multifunctional devices. Here, we demonstrate sizable enhancements of low-frequency dielectric responses in oxygen-deficient oxide ceramics through specific treatments under humid environments. Ultrahigh dielectric permittivity (~5.2 × 106 at 1 Hz) is achieved by hydrogenation, when Ni-substituted BaTiO3 ceramics are exposed to high humidity. Intriguingly, thermal annealing can restore the dielectric on-state (exhibiting huge polarizability in the treated ceramics) to the initial dielectric off-state (displaying low polarizability of ~103 in the pristine ceramics after sintering). The conversion between these two dielectric states via the ambient environment-mediated treatments and the successive application of external stimuli allows us to realize reversible control of dielectric relaxation characteristics in oxide ceramics. Conceptually, our findings are of practical interest for applications to highly efficient dielectric-based humidity sensors.

Reversibly Controlled Ternary Polar States and Ferroelectric Bias Promoted by Boosting Square-Tensile-Strain.

Interaction between dipoles often emerges intriguing physical phenomena, such as exchange bias in the magnetic heterostructures and magnetoelectric effect in multiferroics, which lead to advances in multifunctional heterostructures. However, the defect-dipole tends to be considered the undesired to deteriorate the electronic functionality. Here, deterministic switching between the ferroelectric and the pinched states by exploiting a new substrate of cubic perovskite, BaZrO3 is reported, which boosts the square-tensile-strain to BaTiO3 and promotes four-variants in-plane spontaneous polarization with oxygen vacancy creation. First-principles calculations propose a complex of an oxygen vacancy and two Ti3+ ions coins a charge-neutral defect-dipole. Cooperative control of the defect-dipole and the spontaneous polarization reveals ternary in-plane polar states characterized by biased/pinched hysteresis loops. Furthermore, it is experimentally demonstrated that three electrically controlled polar-ordering states lead to switchable and nonvolatile dielectric states for application of nondestructive electro-dielectric memory. This discovery opens a new route to develop functional materials via manipulating defect-dipoles and offers a novel platform to advance heteroepitaxy beyond the prevalent perovskite substrates.