No Arabic abstract
Materials with reduced dimensions have been shown to host a wide variety of exotic properties and novel quantum states that often defy textbook wisdom1-5. Ferroelectric polarization and metallicity are well-known examples of mutually exclusive properties that cannot coexist in bulk solids because the net electric field in a metal can be fully screened by free electrons6. An atomically thin metallic layer capped by insulating layers has shown decent conductivity at room temperature7. Moreover, a penetrating polarization field can be employed to induce an ion displacement and create an intrinsic polarization in the metallic layer. Here we demonstrate that a ferroelectric metal can be artificially synthesized through imposing a strong polarization field in the form of ferroelectric/unit-cell-thin metal superlattices. In this way the symmetry of an atomically thin conductive layer can be broken and manipulated by a neighboring polar field, thereby forming a two-dimensional (2D) ferroelectric metal. The fabricated of (SrRuO3)1/(BaTiO3)10 superlattices exhibit ferroelectric polarization in an atomically thin layer with metallic conductivity at room temperature. A multipronged investigation combining structural analyses, electrical measurements, and first-principles electronic structure calculations unravels the coexistence of 2D electrical conductivity in the SrRuO3 monolayer accompanied by the electric polarization. Such 2D ferroelectric metal paves a novel way to engineer a quantum multi-state with unusual coexisting properties, such as ferroelectrics, ferromagnetics and metals, manipulated by external fields8,9.
Polar metals, commonly defined by the coexistence of polar crystal structure and metallicity, are thought to be scarce because the long-range electrostatic fields favoring the polar structure are expected to be fully screened by the conduction electrons of a metal. Moreover, reducing from three to two dimensions, it remains an open question whether a polar metal can exist. Here we report on the realization of a room temperature two-dimensional polar metal of the B-site type in tri-color (tri-layer) superlattices BaTiO$_3$/SrTiO$_3$/LaTiO$_3$. A combination of atomic resolution scanning transmission electron microscopy with electron energy loss spectroscopy, optical second harmonic generation, electrical transport, and first-principles calculations have revealed the microscopic mechanisms of periodic electric polarization, charge distribution, and orbital symmetry. Our results provide a route to creating all-oxide artificial non-centrosymmetric quasi-two-dimensional metals with exotic quantum states including coexisting ferroelectric, ferromagnetic, and superconducting phases.
Nanoscaled room-temperature ferroelectricity is ideal for developing advanced non-volatile high-density memories. However, reaching the thin film limit in conventional ferroelectrics is a long-standing challenge due to the possible critical thickness effect. Van der Waals materials, thanks to their stable layered structure, saturate interfacial chemistry and weak interlayer couplings, are promising for exploring ultra-thin two-dimensional (2D) ferroelectrics and device applications. Here, we demonstrate a switchable room-temperature ferroelectric diode built upon a 2D ferroelectric {alpha}-In2Se3 layer as thin as 5 nm in the form of graphene/{alpha}-In2Se3 heterojunction. The intrinsic out-of-plane ferroelectricity of the {alpha}-In2Se3 thin layers is evidenced by the observation of reversible spontaneous electric polarization with a relative low coercive electric field of ~$2 X 10^5 V/cm$ and a typical ferroelectric domain size of around tens ${mu}m^2$. Owing to the out-of-plane ferroelectricity of the {alpha}-In2Se3 layer, the Schottky barrier at the graphene/{alpha}-In2Se3 interface can be effectively tuned by switching the electric polarization with an applied voltage, leading to a pronounced switchable double diode effect with an on/off ratio of ~$10^4$. Our results offer a new way for developing novel nanoelectronic devices based on 2D ferroelectrics.
The advent of long-range magnetic order in non-centrosymmetric compounds has stimulated interest in the possibility of exotic spin transport phenomena and topologically protected spin textures for applications in next-generation spintronics. This work reports a novel wurtzite-structure polar magnetic metal, identified as AA-stacked (Fe0.5Co0.5)5-xGeTe2, which exhibits a Neel-type skyrmion lattice as well as a Rashba-Edelstein effect at room temperature. Atomic resolution imaging of the structure reveals a structural transition as a function of Co-substitution, leading to the polar phase at 50% Co. This discovery reveals an unprecedented layered polar magnetic system for investigating intriguing spin topologies and ushers in a promising new framework for spintronics.
Integrating multiple properties in a single system is crucial for the continuous developments in electronic devices. However, some physical properties are mutually exclusive in nature. Here, we report the coexistence of two seemingly mutually exclusive properties-polarity and two-dimensional conductivity-in ferroelectric Ba$_{0.2}$Sr$_{0.8}$TiO$_3$ thin films at the LaAlO$_3$/Ba$_{0.2}$Sr$_{0.8}$TiO$_3$ interface at room temperature. The polarity of a ~3.2 nm Ba$_{0.2}$Sr$_{0.8}$TiO$_3$ thin film is preserved with a two-dimensional mobile carrier density of ~0.05 electron per unit cell. We show that the electronic reconstruction resulting from the competition between the built-in electric field of LaAlO$_3$ and the polarization of Ba$_{0.2}$Sr$_{0.8}$TiO$_3$ is responsible for this unusual two-dimensional conducting polar phase. The general concept of exploiting mutually exclusive properties at oxide interfaces via electronic reconstruction may be applicable to other strongly-correlated oxide interfaces, thus opening windows to new functional nanoscale materials for applications in novel nanoelectronics.
Ferroelectric materials contain a switchable spontaneous polarization that persists even in the absence of an external electric field. The coexistence of ferroelectricity and metallicity in a material appears to be illusive, since polarization is ill-defined in metals, where the itinerant electrons are expected to screen the long-range dipole interactions necessary for dipole ordering. The surprising discovery of the polar metal, LiOsO3 has generated interest in searching for new polar metals motivated by the prospects of exotic quantum phenomena such as unconventional pairing mechanisms giving rise to superconductivity, topological spin currents, anisotropic upper critical fields, and Mott multiferroics. Previous studies have suggested that the coordination preferences of the Li atom play a key role in stabilizing the polar metal phase of LiOsO3, but a thorough understanding of how polar order and metallicity can coexist remains elusive. Here, we use XUV-SHG as novel technique to directly probe the broken inversion-symmetry around the Li atom. Our results agree with previous theories that the primary structural distortion that gives rise to the polar metal phase in LiOsO3 is a consequence of a sub-Angstrom Li atom displacement along the polar axis. A remarkable agreement between our experimental results and ab initio calculations provide physical insights for connecting the nonlinear response to unit-cell spatial asymmetries. It is shown that XUV-SHG can selectively probe inversion-breaking symmetry in a bulk material with elemental specificity. Compared to optical SHG methods, XUV-SHG fills a key gap for studying structural asymmetries when the structural distortion is energetically separated from the Fermi surface. Further, these results pave the way for time-resolved probing of symmetry-breaking structural phase transitions on femtosecond timescales with element specificity.