Hexagonal Rare-Earth Manganites as Promising Photovoltaics and Light Polarizers

Ferroelectric materials possess a spontaneous electric polarization and may be utilized in various technological applications ranging from non-volatile memories to solar cells and light polarizers. Recently, hexagonal rare-earth manganites, h-RMnO$_3$ (R is a rare-earth ion) have attracted considerable interest due to their intricate multiferroic properties and improper ferroelectricity characterized by a sizable remnant polarization and high Curie temperature. Here, we demonstrate that these compounds can serve as very efficient photovoltaic materials and, in addition, possess remarkable optical anisotropy properties. Using first-principles methods based on density-functional theory and considering h-TbMnO$_3$ as a representative manganite, we predict a strong light absorption of this material in the solar spectrum range, resulting in the maximum light-to-electricity energy conversion efficiency up to 33%. We also predict an extraordinary optical linear dichroism and linear birefringence properties of h-TbMnO$_3$ in a broad range of optical frequencies. These results uncover the unexplored potential of hexagonal rare-earth manganites to serve as photovoltaics in solar cells and as absorptive and birefringent light polarizers.Comment: 26 pages, 8 figure

Prediction of a mobile two-dimensional electron gas at the LaScO3/BaSnO3(001) interface

Two-dimensional electron gases (2DEG) at oxide interfaces, such as LaAlO3/SrTiO3 (001), have aroused significant interest due to their high carrier density (∼1014 cm−2) and strong lateral confinement (∼1 nm). However, these 2DEGs are normally hosted by the weakly dispersive and degenerate d bands (e.g., Ti-3d bands), which are strongly coupled to the lattice, causing mobility of such 2DEGs to be relatively low at room temperature (∼1 cm2/Vs). Here, we propose using oxide host materials with the conduction bands formed from s electrons to increase carrier mobility and soften its temperature dependence. Using first-principles density functional theory calculations, we investigate LaScO3/BaSnO3 (001) heterostructure and as a model system, where the conduction band hosts the s-like carriers. We find that the polar discontinuity at this interface leads to electronic reconstruction resulting in the formation of the 2DEG at this interface. The conduction electrons reside in the highly dispersive Sn-5s bands, which have a large band width and a low effective mass. The predicted 2DEG is expected to be highly mobile even at room temperature due to the reduced electron-phonon scattering via the inter-band scattering channel. A qualitatively similar behavior is predicted for a doped BaSnO3, where a monolayer of BaO is replaced with LaO. We anticipate that the quantum phenomena associated with these 2DEGs to be more pronounced owing to the high mobility of the carriers

Effects of intermixing and oxygen vacancies on a two-dimensional electron gas at the polar (TbScO\u3csub\u3e3\u3c/sub\u3e/KTaO) (001) interface

3d-5d perovskite oxides, ABO3 (where A and B are 3d or 5d elements), form polar surfaces in the (001)- stacked thin films. As a result, the polar-polar (001) interface between two ABO3 insulators could create polar discontinuity potentially producing a two-dimensional electron gas of higher density and stronger spatial localization compared to the widely studied polar-nonpolar oxide interfaces, such as (001) LaAlO3/SrTiO3. Here, as a model system, we explore the interface between polar (001) TbScO3 and polar (001) KTaO3 using first-principles density functional theory.We find that the intermixed interface Ta0.75Sc0.25O2/Tb0.75K0.25O maintaining the bulk perovskite charge stacking (e.g., . . . + 1/ − 1/ + 1 . . .) is insulating and has a lower energy than the metallic interface TbO/TaO2 breaking such stacking. This intermixed interface is, however, prone to the formation of oxygen vacancies which make it conducting. We emphasize that the driving force for the formation of the two-dimensional electron gas (2DEG) here is not a built-in electric field stemming from the polar discontinuity but the interface stoichiometry. We find that the ratio of oxygen vacancy concentration is a factor of 30 times larger at the interface than in bulk KTO at room temperature. The oxygen vacancy-induced 2DEG resides on the Ta-5d electronic orbitals with dxy and dxz/yz occupation dominating overall charge density near and far away from the interface

Hexagonal rare-earth manganites as promising photovoltaics and light polarizers

Ferroelectric materials possess a spontaneous electric polarization and may be utilized in various technological applications ranging from nonvolatile memories to solar cells and light polarizers. Recently, hexagonal rareearth manganites, h-RMnO3 (R is a rare-earth ion), have attracted considerable interest due to their intricate multiferroic properties and improper ferroelectricity characterized by a sizable remnant polarization and high Curie temperature. Here we demonstrate that these compounds can serve as very efficient photovoltaic materials and, in addition, possess remarkable optical anisotropy properties. Using first-principles methods based on density functional theory and considering h-TbMnO3 as a representative manganite, we predict a strong light absorption of this material in the solar spectrum range, resulting in a maximum light-to-electricity energy conversion efficiency of up to 33%. We also predict an extraordinary optical linear dichroism and linear birefringence properties of h-TbMnO3 in a broad range of optical frequencies. These results uncover the unexplored potential of hexagonal rare-earth manganites to serve as photovoltaics in solar cells and as absorptive and birefringent light polarizers

Reversible spin texture in ferroelectric HfO\u3csub\u3e2\u3c/sub\u3e

Spin-orbit coupling effects occurring in noncentrosymmetric materials are known to be responsible for nontrivial spin configurations and a number of emergent physical phenomena. Ferroelectric materials may be especially interesting in this regard due to reversible spontaneous polarization making possible a nonvolatile electrical control of the spin degrees of freedom. Here, we explore a technologically relevant oxide material, HfO2, which has been shown to exhibit robust ferroelectricity in a noncentrosymmetric orthorhombic phase. Using theoretical modelling based on density-functional theory, we investigate the spin-dependent electronic structure of the ferroelectric HfO2 and demonstrate the appearance of chiral spin textures driven by spin-orbit coupling. We analyze these spin configurations in terms of the Rashba and Dresselhaus effects within the k · p Hamiltonian model and find that the Rashba-type spin texture dominates around the valence-band maximum, while the Dresselhaus-type spin texture prevails around the conduction band minimum. The latter is characterized by a very large Dresselhaus constant λD = 0.578 eV A, which allows using this material as a tunnel barrier to ˚ produce tunneling anomalous and spin Hall effects that are reversible by ferroelectric polarization

Anomalous Hall Conductivity of a Non-Collinear Magnetic Antiperovskite

The anomalous Hall effect (AHE) is a well-known fundamental property of ferromagnetic metals, commonly associated with the presence of a net magnetization. Recently, an AHE has been discovered in non-collinear antiferromagnetic (AFM) metals. Driven by non-vanishing Berry curvature of AFM materials with certain magnetic space group symmetry, anomalous Hall conductivity (AHC) is very sensitive to the specific type of magnetic ordering. Here, we investigate the appearance of AHC in antiperovskite GaNMn$_{3}$ as a representative of broader materials family ANMn$_{3}$ (A is a main group element), where different types of non-collinear magnetic ordering can emerge. Using symmetry analyses and first-principles density-functional theory calculations, we show that with almost identical band structure, the nearly degenerate non-collinear AFM $\Gamma_{5g}$ and $\Gamma_{4g}$ phases of GaNMn$_{3}$ have zero and finite AHC, respectively. In a non-collinear ferrimagnetic $M$-1 phase, GaNMn$_{3}$ exhibits a large AHC due to the presence of a sizable net magnetic moment. In the non-collinear antiperovskite magnets, transitions between different magnetic phases, exhibiting different AHC states, can be produced by doping, strain, or spin transfer torque, which makes these materials promising for novel spintronic applications

Spin-polarized two-dimensional electron gas at GdTiO3/SrTiO3 interfaces: Insight from first-principles calculations

Two-dimensional electron gases (2DEGs) at oxide interfaces have been a topic of intensive research due to their high carrier mobility and strong confinement. Additionally, strong correlations in the oxide materials can give rise to new and interesting physics, such as magnetism and metal-insulator transitions at the interface. Using first-principles calculations based on density functional theory, we demonstrate the presence of a highly spin-polarized 2DEG at the interface between the Mott insulator GdTiO3 and a band insulator SrTiO3. The strong correlations in the dopant cause ferromagnetic alignment of the interface Ti atoms and result in a fully spin-polarized 2DEG. The 2DEG consists of two types of carriers distinguished by their orbital character. The majority of the interface charge is strongly localized on the Ti dxy orbitals at the interface and a smaller fraction resides on the delocalized Ti dxz,yz states

Anomalous Hall conductivity of noncollinear magnetic antiperovskites

The anomalous Hall effect (AHE) is a well-known fundamental property of ferromagnetic metals, commonly associated with the presence of a net magnetization. Recently, an AHE has been discovered in noncollinear antiferromagnetic (AFM) metals. Driven by nonvanishing Berry curvature of AFM materials with certain magnetic space-group symmetry, anomalous Hall conductivity (AHC) is very sensitive to the specific type of magnetic ordering. Here, we investigate the appearance of AHC in antiperovskite materials family ANMn3 (A = Ga, Sn, Ni), where different types of noncollinear magnetic ordering can emerge. Using symmetry analyses and first-principles density-functional theory calculations, we show that with almost identical band structure the nearly degenerate noncollinear AFM Γ5g and Γ4g phases of GaNMn3 have zero and finite AHC, respectively. In a noncollinear ferrimagnetic M-1 phase, GaNMn3 exhibits a large AHC due to the presence of a sizable net magnetic moment. In the noncollinear antiperovskite magnets, transitions between different magnetic phases, exhibiting different AHC states, can be produced by doping, strain, or spin transfer torque, which makes these materials promising for novel spintronic applications

Reversible spin texture in ferroelectric HfO2

Spin-orbit coupling effects occurring in non-centrosymmetric materials are known to be responsible for non-trivial spin configurations and a number of emergent physical phenomena. Ferroelectric materials may be especially interesting in this regard due to reversible spontaneous polarization making possible for a non-volatile electrical control of the spin degrees of freedom. Here, we explore a technologically relevant oxide material, HfO2, which has been shown to exhibit robust ferroelectricity in a non-centrosymmetric orthorhombic phase. Using theoretical modelling based on density-functional theory, we investigate the spin-dependent electronic structure of the ferroelectric HfO2 and demonstrate the appearance of chiral spin textures driven by spin-orbit coupling. We analyze these spin configurations in terms of the Rashba and Dresselhaus effects within the k.p Hamiltonian model and find that the Rashba-type spin texture dominates around the valence band maximum, while the Dresselhaus-type spin texture prevails around the conduction band minimum. The latter is characterized by a very large Dresselhaus constant {\alpha}D = 0.578 eV {\AA}, which allows using this material as a tunnel barrier to produce tunneling anomalous and spin Hall effects that are reversible by ferroelectric polarization