Antiferromagnetic thin films typically exhibit a multi-domain state, and control of the antiferromagnetic Néel vector is challenging as antiferromagnetic materials are robust to magnetic perturbations. By relying on anisotropic in-plane strain engineering of epitaxial thin films of the prototypical antiferromagnetic material LaFeO3, uniaxial Néel vector control is demonstrated. Orthorhombic (011)- and (101)-oriented DyScO3, GdScO3 and NdGaO3 substrates are used to engineer different anisotropic in-plane strain states. The anisotropic in-plane strain stabilises structurally monodomain monoclinic LaFeO3 thin films. The uniaxial Néel vector is found along the tensile strained b axis, contrary to bulk LaFeO3 having the Néel vector along the shorter a axis, and no magnetic domains are found. Hence, anisotropic strain engineering is a viable tool for designing unique functional responses, further enabling antiferromagnetic materials for mesoscopic device technology.
Persistent spin textures are highly desirable for applications in spintronics as they may allow for long carrier spin lifetimes. However, they are also rare as only four point groups can host such textures, and even for these four groups, the emergence of persistent spin textures requires a delicate balance between coupling parameters, which control the strength of spin-momentum interactions. We use first-principles density functional simulations to predict the possibility of achieving these desirable spin textures through the application of uniaxial stress. Hybrid organic-inorganic perovskite…
The structural, elastic, magnetic properties, as well as electronic structure and chemical bonding picture of new oxide 3d1-perovskite BaVO3, recently synthesized, were systematically investigated involving the first-principles FLAPW-GGA calculations. The obtained results are discussed in comparison with available experimental data, as well as with those obtained before for isostructural and isoelectronic SrVO3 perovskite.
The energetics of vicinal SrTiO$_3$(001) and DyScO$_3$(110), prototypical perovskite vicinal surfaces, has been studied using topographic atomic force microscopy imaging. The kink formation and strain relaxation energies are extracted from a statistical analysis of the step meandering. Both perovskite surfaces have very similar kink formation energies and exhibit a similar triangular step undulation. Our experiments suggest that the energetics of perovskite oxide surfaces is mainly governed by the local oxygen coordination.
ABO3 oxides with the perovskite-related structures are attracting significant interest due to their promising physical and chemical properties for many applications requiring tunable chemistry, including fuel cells, catalysis, and electrochemical water splitting. Here we report on the crystal structure of the entire family of perovskite oxides with ABO3 stoichiometry, where A and B are Ba, Sr, Mn, Ce. Given the vast size of this chemically complex material system, exploration for stable perovskite-related structures with respect to its constituent elements and annealing temperature is performe…
We perform first-principles density functional calculations to explore the role of substrate proximity effects on the octahedral rotation patterns in perovskite oxide superlattices. With cubic perovskite SrFeO$_3$ as our model film and tetragonal SrTiO$_3$ as the substrate, we show that in most cases the substrate octahedral rotation patterns propagate into the film across the heterointerface. We also identify elastic boundary conditions for which the enforced structural coherence induces atomic displacement patterns that are not found in the bulk phase diagram of either individual constituent…
The discovery of two-dimensional electron gases (2DEGs) at the heterointerface between two insulating perovskite-type oxides, such as LaAlO3 and SrTiO3, provides opportunities for a new generation of all-oxide electronic and photonic devices. However, significant improvement of the interfacial electron mobility beyond the current value of approximately 1,000 cm2V-1s-1 (at low temperatures), remains a key challenge for fundamental as well as applied research of complex oxides. Here, we present a new type of 2DEG created at the heterointerface between SrTiO3 and a spinel γ-Al2O3 epitaxial film w…
Perovskite oxides exhibit a rich variety of structural phases hosting different physical phenomena that generate multiple technological applications. We find that topological phonons, i.e., nodal rings, nodal lines, and Weyl points, are ubiquitous in oxide perovskites in terms of structures (tetragonal, orthorhombic, and rhombohedral), compounds (BaTiO3, PbTiO3, and SrTiO3), and external conditions (photoexcitation, strain, and temperature). In particular, in the tetragonal phase of these compounds, all types of topological phonons can simultaneously emerge when stabilized by photoexcitation, …
We report calculations indicating that amorphous RAO$_3$ oxides, with R and A trivalent cations, have approximately the same static dielectric constant as their perovskite crystal phase. The effect is due to the disorder-activated polar response of non-polar crystal modes at low frequency, which compensates a moderate but appreciable reduction of the ionic dynamical charges. The dielectric response was studied via density-functional perturbation theory. Amorphous samples were generated by molecular dynamics melt-and-quench simulations.
Transition-metal perovskite oxides constitute a series of functional material systems for electronics, catalysis and energy-conversion processes, in which oxygen migration and evolution play a key role. However, the stable metal-oxygen (M-O) bond forms large energy barrier inhibiting ion diffusion. Therefore, seeking efficient and facile approaches to accelerate oxygen kinetics has become a significant issue. Here, the interaction (interfacial charge transfer and cooperative bonding) between noble metal (Pt, Ag) and perovskites oxide (SrCoO3-delta) is employed to weaken (M-O) bond and decrease…
The optimization of properties of perovskite oxides has drawn interest on account of their diverse areas of application. In this work, the hierarchical clustering technique is used to reduce the multi-collinearity among selected features from literature that are reported to have an effect on perovskite formation and stability. Operating on the vast composition space of double oxide perovskite compositions available in literature and online repositories, in this manuscript, an attempt has been made to extract the relationship between the composition and structure to predict their formability an…
Two-dimensional (2D) materials are able to strongly confine light hybridized with collective excitations of atoms, enabling electric-field enhancements and novel spectroscopic applications. Recently, freestanding monolayers of oxide perovskites have been synthesized, which possess highly infrared-active phonon modes and a complex interplay of competing interactions. In this study, we evaluate central figures of merit for phonon polaritons in the tetragonal phases of the 2D perovskites SrTiO$_3$, KTaO$_3$, and LiNbO$_3$, using density functional theory calculations. Specifically, we compute the…
This article reviews the polarizability model and its applications to ferroelectric perovskite oxides. The motivation for the introduction of the model is discussed and nonlinear oxygen ion polarizability effects and their lattice dynamical implementation outlined. While a large part of this work is dedicated to results obtained within the self-consistent-phonon approximation (SPA), also nonlinear solutions of the model are handled which are of interest to the physics of relaxor ferroelectrics, domain wall motions, incommensurate phase transitions. The main emphasis is to compare the results o…
In this comment to [S. Lenjer, O. F. Schirmer, H. Hesse, and Th. W. Kool, Phys. Rev. B {\bf 66}, 165106 (2002)] we discuss the electronic structure of oxygen vacancies in perovskites. First principles computations are in favour of rather deep levels in these vacancies, and Lenjer et al suggest that the electrons' interaction energy is negative, but data on electroconductivity are against.
Using a CO$_2$ laser to directly heat the crystals from the back side, SrTiO$_3$ substrates may be thermally prepared in situ for epitaxy without the need for ex-situ etching and annealing. We find that the formation of large terraces with straight steps at 900-1100 °C is independent from the formation of the ideal surface reconstruction for epitaxy, which requires temperatures in excess of 1200 °C to complete. The process may be universal, at least for perovskite oxide surfaces, as it also works, at different temperatures, for LaAlO$_3$ and NdGaO$_3$, two other widely used oxide substrate mat…
The use of microwave irradiation is a promising alternative heat source for the synthesis of inorganic materials such as perovskite oxides. The method offers massive energy and time savings as compared to the traditional ceramic method. In this work we review the basic principles of the microwave heating mechanism based on interactions between dipoles in the material and the electromagnetic microwave. Furthermore, we comment on and classify all different sub-types of microwave synthesis such as solid-state microwave and microwave assisted hydrothermal synthesis. In the experimental part of thi…
Perovskite transition-metal oxides are networks of corner-sharing octahedra whose tilts and distortions are known to affect their electronic and magnetic properties. We report calculations on a model interfacial structure to avoid chemical influences and show that the symmetry mismatch imposes an interfacial layer with distortion modes that do not exist in either bulk material, creating new interface properties driven by symmetry alone. Depending on the resistance of the octahedra to deformation, the interface layer can be as small as one unit cell or extend deep into the thin film.
There are two silver perovskite oxides: AgNbO3 and AgTaO3. AgNbO3 has a noncentrosymmetric group of Pmc21 at room temperature with a ferri-electric ordering of polarization. Such a ferri-electric state with small polarization can be changed into a ferroelectric state with very large polarization by a high electric field or by a chemical modification. The induced ferroelectric phase shows promising electromechanical response for applications in piezoelectric devices. In contrast, AgTaO3 is a quantum paraelectric, but ferroelectricity also can be induced through chemical substitution. The findin…
We present an aberration corrected scanning transmission electron microscopy (ac-STEM) analysis of the perovskite (LaFeO3) and pyrochlore (Yb2Ti2O7 and Pr2Zr2O7) oxides and demonstrate that both the shape and contrast of visible atomic columns in annular dark-field (ADF) images are sensitive to the presence of nearby atoms of low atomic number (e.g. oxygen). We show that point defects (e.g. oxygen vacancies), which are invisible - or difficult to observe due to limited sensitivity - in X-ray and neutron diffraction measurements, are the origin of the complex magnetic ground state of pyrochlore…
Perovskite photovoltaics (PVs) have attracted attention because of their excellent power conversion efficiency (PCE). Critical issues related to large area PV performance, reliability and lifetime need to be addressed. Here, we show that doped metal oxides can provide ideal electron selectivity, improved reliability and stability for perovskite PVs. We report p-i-n perovskite PVs with device areas ranging from 0.09cm2 to 0.5cm2 incorporating a thick aluminum doped zinc oxide (AZO) electron selective contact with hysteresis-free PCE of over 13% and high fill factor values in the range of 80%. A…
Vacancy defects in thin film laser ablated SrTiO3 on SrTiO3 were identified using variable energy positron annihilation lifetime measurements. Strontium vacancy related defects were the dominant positron traps and, apart from in the top ~ 50 nm, were found to be uniformly distributed. The surface layer showed an increase in annihilation from larger open-volume defects, large vacancy clusters or nanovoids.
Thin films of perovskite oxides offer the possibility of combining emerging concepts of strongly correlated electron phenomena and spin current in magnetic devices. However, spin transport and magnetization dynamics in these complex oxide materials are not well understood. Here, we experimentally quantify spin transport parameters and magnetization damping in epitaxial perovskite ferromagnet/paramagnet bilayers of La$_{2/3}$Sr$_{1/3}$MnO$_3$/SrRuO$_3$ (LSMO/SRO) by broadband ferromagnetic resonance spectroscopy. From the SRO thickness dependence of Gilbert damping, we estimate a short spin dif…
The band offsets for nine heterojunctions between titanates, zirconates, and niobates with the cubic perovskite structure were calculated from first principles. The effect of strain in contacting oxides on their energy structure, many-body corrections to the position of the band edges (calculated in the GW approximation), and the splitting of the conduction band resulting from spin-orbit interaction were consistently taken into account. It was shown that the neglect of the many-body effects can lead to errors in determination of the band offsets up to 0.36 eV. The failure of the transitivity r…
Predicting the stability of the perovskite structure remains a longstanding challenge for the discovery of new functional materials for many applications including photovoltaics and electrocatalysts. We developed an accurate, physically interpretable, and one-dimensional tolerance factor, τ, that correctly predicts 92% of compounds as perovskite or nonperovskite for an experimental dataset of 576 $ABX_3$ materials ($\textit{X} =$ $O^{2-}$, $F^-$, $Cl^-$, $Br^-$, $I^-$) using a novel data analytics approach based on SISSO (sure independence screening and sparsifying operator). τ is shown to gen…
We predict through our first-principles calculations that four double perovskite oxides of Bi2ABO6 (AB = FeMo, MnMo, MnOs, CrOs) are half-metallic ferrimagnets. Our calculated results shows that the four optimized structures have negative formation energy, from -0.42 to -0.26 eV per formula unit, which implies that they could probably be realized. In the case of Bi2FeMoO6, the half-metallic gap and Curie temperature are predicted to reach to 0.71 eV and 650 K, respectively, which indicates that high spin polarization could be kept at high temperatures far beyond room temperature. It is believe…
In the present paper, the electronic, structural, thermodynamic, and elastic properties of cubic $PbGeO_{3}$ perovskite oxide are presented and computed using the WIEN2K code. The structural properties have been evaluated and they are in good agreement with the theoretical and experimental data. A phonon dispersion is made and it reveals that the cubic $PbGeO_{3}$ perovskite is dynamically stable. In addition, the electronic properties of $PbGeO_{3}$ shows an opening gap energy, meaning a semiconductor behavior with an indirect band gap equal to $1.67 eV$. Moreover, the obtained elastic consta…
Tuning the work functions of materials is of practical interest for maximizing the performance of microelectronic and (photo)electrochemical devices, as the efficiency of these systems depends on the ability to control electronic levels at surfaces and across interfaces. Perovskites are promising compounds to achieve such control. In this work, we examine the work functions of more than 1,000 perovskite oxide surfaces (ABO$_3$) by data-driven (machine-learning) analysis and identify the factors that determine their magnitude. While the work functions of BO$_2$-terminated surfaces are sensitive…
Ferromagnetic insulators (FMIs) are one of the most important components in developing dissipationless electronic and spintronic devices. However, since ferromagnetism generally accompanies metallicity, FMIs are innately rare to find in nature. Here, novel room-temperature FMI films are epitaxially synthesized by deliberate control of the ratio of two B-site cations in the double perovskite Sr2FeReO6. In contrast to the known ferromagnetic metallic phase in stoichiometric Sr2FeReO6, a FMI state with a high Curie temperature (Tc~400 K) and a large saturation magnetization (MS~1.8 μB/f.u.) is fo…
High entropy oxides (HEO) are a recently introduced class of oxide materials, which are characterized by a large number of elements (i.e. five or more) sharing one lattice site which crystallize in a single phase structure. One complex example of the rather young HEO family are the rare-earth transition metal perovskite high entropy oxides. In this comprehensive study, we provide an overview over the magnetic properties of three perovskite type high entropy oxides. The compounds have a rare-earth site which is occupied by five different rare-earth elements, while the transition metal site is o…
Symbolic regression (SR) is an emerging method for building analytical formulas to find models that best fit data sets. Here, SR was used to guide the design of new oxide perovskite catalysts with improved oxygen evolution reaction (OER) activities. An unprecedentedly simple descriptor, μ/t, where μ and t are the octahedral and tolerance factors, respectively, was identified, which accelerated the discovery of a series of new oxide perovskite catalysts with improved OER activity. We successfully synthesized five new oxide perovskites and characterized their OER activities. Remarkably, four of …
An ab initio structure optimization technique is newly developed to determine the valley line on a total-energy surface for zone-center distortions of ferroelectric perovskite oxides and is applied to barium titanate BaTiO3 and lead titanate PbTiO3. The proposed technique is an improvement over King-Smith and Vanderbilt's scheme [Phys. Rev. B 49, p.5828 (1994)] of evaluating total energy as a function of the amplitude of atomic displacements. The results of numerical calculations show that total energy can be expressed as a fourth-order function of the amplitude of atomic displacements in BaTi…
Sodium iridium(V) oxide, NaIrO3, was synthesized by a high pressure solid state method and recovered to ambient conditions. It is found to be isostructural with CaIrO3, the much-studied structural analogue of the high-pressure post-perovskite phase of MgSiO3. Among the oxide post-perovskites, NaIrO3 is the first example with a pentavalent cation. The structure consists of layers of corner- and edge-sharing IrO6 octahedra separated by layers of NaO8 bicapped trigonal prisms. NaIrO3 shows no magnetic ordering and resistivity measurements show non-metallic behavior. The crystal structure, electri…
Strain engineering with different substrate facets is promising for tuning functional properties of thin film perovskite oxides. By choice of facet, different surface symmetries and chemical bond directions for epitaxial interfaces can be tailored. Here, preparation of well-defined pseudo-cubic (111)-oriented orthorhombic substrates of DyScO3 , GdScO3 , and NdGaO3 is reported. The choice of orthorhombic facet, (011)o or (101)o , both corresponding to pseudo-cubic (111)pc , gives vicinal surfaces with single or double (111pc layer terrace step heights, respectively, impacting subsequent thin fi…
In transition metal perovskites (ABO3) most physical properties are tunable by structural parameters such as the rotation of the BO6 octahedra. Examples include the Néel temperature of orthoferrites, the conductivity of mixed-valence manganites, or the band gap of rare-earth scandates. Since oxides often host large internal electric dipoles and can accommodate heavy elements, they also emerge as prime candidates to display Rashba spin-orbit coupling, through which charge and spin currents may be efficiently interconverted. However, despite a few experimental reports in SrTiO3-based interface s…
We propose a device model that elucidates the role of domain walls in the photovoltaic effect in multi-domain ferroelectric perovskites. The model accounts for the intricate interplay between ferroelectric polarization, space charges, photo-generation and electronic transport. When applied to bismuth ferrite, results show a significant electric potential step across both 71-degree and 109-degree domain walls, which in turn contributes to the photovoltaic (PV) effect. We also find a strong correlation between polarization and oxygen octahedra tilts, which indicates the nontrivial role of the la…
Oxide materials exhibit several novel structural, magnetic, and electronic properties. Their stability under ambient conditions, easy synthesis, and high transition temperatures provide such systems with an ideal ground for realizing topological properties and real-life technological applications. However, experimental evidence of topological states in oxide materials is rare. In this study, we have synthesized single crystals of oxide double perovskite Sr2FeMoO6 and revealed its topological nature by investigating its structural, magnetic, and electronic properties. We observed that the syste…
The momentum-dependent Rashba and Dresselhaus spin-splitting has gained much attention for its highly promising applications in spintronics. In the present work, ab initio density functional theory calculations are performed to study the spin-splitting effect in ferroelectric oxide perovskite KIO3. Our calculations are additionally supported by symmetry adapted two-band k.p Hamiltonian. Non-negligible spin-splitting effect is observed at conduction band minimum (CBm) and valence band maximum (VBM) for rhombohedral R3m and R3c phases. Linear Rashba terms successfully explain the splitting at VB…
Mixed oxides derived from the perovskite structure by combination of A- and B-site elements and by partial substitution of oxygen provide an immense playground of physico-chemical properties. Here, we account for own research conducted at the Paul Scherrer Institute on perovskite-type oxides and oxynitrides used in electrochemical, photo(electro)chemical and catalytic processes aiming at facing energy relevant issues.
We report a study on the interface between polar high-k materials and the Si(001)-(2X1) reconstructed surface with LaAlO3 taken as a prototype material. The construction of the interface is based on the prior growth of metal lines followed by oxidation, whose stability against oxygen coverage is studied. Electronic structure calculations within the Density Functional Theory framework help in building the interface and understanding its bonding structure. Moreover, we computed a conduction band offset of 1.9 eV, in agreement with electronic applications requirement. The results may provide a gu…
Perovskite materials have become ubiquitous in many technologically relevant applications, ranging from catalysts in solid oxide fuel cells to light absorbing layers in solar photovoltaics. The thermodynamic phase stability is a key parameter that broadly governs whether the material is expected to be synthesizable, and whether it may degrade under certain operating conditions. Phase stability can be calculated using Density Functional Theory (DFT), but the significant computational cost makes such calculation potentially prohibitive when screening large numbers of possible compounds. In this …
Recent realizations of ultrathin freestanding perovskite oxides offer a unique platform to probe novel properties in two-dimensional oxides. Here, we observed a giant flexoelectric response in freestanding BiFeO3 and SrTiO3 in their bent state arising from strain gradients up to 4x10e7/m, suggesting a promising approach for realizing extremely large polarizations. Additionally, a substantial reversible change in thickness was discovered in bent freestanding BiFeO3, which implies an unusual bending-expansion/shrinkage and thickness-dependence Poisson's ratios in this ferroelectric membrane that…
Spin-phonon interactions are central to many interesting phenomena, ranging from superconductivity to magnetoelectric effects. Yet, they are believed to have a negligible influence on the structural behavior of most materials. For example, magnetic perovskite oxides often undergo structural transitions accompanied by magnetic signatures whose minuteness suggests that the underlying spin-phonon couplings are largely irrelevant. Here we present an exception to this rule, showing that novel effects can occur as a consequence. Our first-principles calculations reveal that spin-phonon interactions …
Oxide electronics relies on the availability of epitaxial oxide thin films. The extreme flexibility of the chemical composition of ABO3 perovskites and the broad spectrum of properties they cover, inspire the creativity of scientists and place perovskites in the lead of functional materials for advanced technologies. Moreover, emerging properties are being discovered at interfaces between distinct perovskites that could not be anticipated on the basis of those of the adjacent epitaxial layers. All dreamed new prospects require the use of suitable substrates for epitaxial growth. Perovskite sin…
We used first-principles calculations to investigate the existence and origin of the ferroelectric in- stability in the ABF3 fluoro-perovskites. We find that many fluoro-perovskites have a ferroelectric instability in their high symmetry cubic structure, which is of similar amplitude to that commonly found in oxide perovskites. In contrast to the oxides, however, the fluorides have nominal Born effective charges, indicating a different mechanism for the instability. We show that the instability originates from ionic size effects, and is therefore in most cases largely insensitive to pressure a…
We investigate the structure--property relationships in $AB$O$_3$ perovskites exhibiting octahedral rotations and cooperative octahedral breathing distortions (CBD) using group theoretical methods. Rotations of octahedra are ubiquitous in the perovskite family, while the appearance of breathing distortions -- oxygen displacement patterns that lead to approximately uniform dilation and contraction of the $B$O$_6$ octahedra -- are rarer in compositions with a single, chemically unique $B$-site. The presence of a CBD relies on electronic instabilities of the $B$-site cations, either orbital degen…
Using finite-temperature phonon calculations and the Lyddane-Sachs-Teller relations, we calculate ab initio the static dielectric constants of 78 semiconducting oxides and fluorides with cubic perovskite structures at 1000 K. We first compare our method with experimental measurements, and we find that it succeeds in describing the temperature dependence and the relative ordering of the static dielectric constant $ε_{DC}$ in the series of oxides BaTiO$_{3}$, SrTiO$_{3}$, KTaO$_{3}$. We show that the effects of anharmonicity on the ion-clamped dielectric constant, on Born charges, and on phonon …
Our first-principles results show that geometric frustration can be induced in thin films of multiferroic BiFeO3. We find that competing magnetic interactions occur in the so-called super-tetragonal phase of this material, which can be grown on strongly-compressive substrates. We show that the frustration level can be tuned by appropriately choosing the substrate; in fact, the three-dimensional spin order gets totally annihilated in a narrow range of epitaxial strains. We argue that the effects revealed here are not exclusive to BiFeO3, and predict that they also occur in multiferroic BiCoO3.
The oxygen evolution reaction (OER) is considered a key reaction for electrochemical energy conversion but slow kinetics hamper application in electrolyzers, metal-air batteries and other applications that rely on sustainable protons from water oxidation. In this review, the prospect of epitaxial perovskite oxides for the OER at room temperature in alkaline media is reviewed with respect to fundamental insight into systematic trends of the activity. First, we thoroughly define the perovskite structure and its parameter space. Then, the synthesis methods used to make electrocatalytic epitaxial …
Magnetic insulators with strong perpendicular magnetic anisotropy (PMA) play a key role in exploring pure spin current phenomena and developing ultralow-dissipation spintronic devices, thereby it is highly desirable to develop new material platforms. Here we report epitaxial growth of La2/3Sr1/3MnO3 (LSMO)-SrIrO3 (SIO) composite oxide films (LSMIO) with different crystalline orientations fabricated by sequential two-target ablation process using pulsed laser deposition. The LSMIO films exhibit high crystalline quality with homogeneous mixture of LSMO and SIO at atomic level. Ferrimagnetic and …
We report a theoretical study of the non-linear magnetoelectric response of GdFeO$_3$ through an analytical approach combined with a Heisenberg model which is fitted against first-principles calculations. Our theory reproduces the non-linear change of polarization under applied magnetic field reported experimentally such that it allows to analyze the origin of the large responses in the different directions. We show that the non-linear character of the response in these materials originates from the fact that the antiferromagnetic order of Gd atoms changes non-linearly with respect to the appl…
Critical to the development of improved solid oxide fuel cell (SOFC) technology are novel compounds with high oxygen reduction reaction (ORR) catalytic activity and robust stability under cathode operating conditions. Approximately 2145 distinct perovskite compositions are screened for potential use as high activity, stable SOFC cathodes, and it is verified that the screening methodology qualitatively reproduces the experimental activity, stability, and conduction properties of well-studied cathode materials. The calculated oxygen p-band center is used as a first principle-based descriptor of …
Two-dimensional (2D) ferroelectricity has attracted extensive attention since its discovery in the monolayers of van der Waals materials. Here we show that 2D ferroelectricity induced by octahedral rotation distortion is widely present in the perovskite bilayer system through first-principles calculations. The perovskite tolerance factor plays a crucial role in the lattice dynamics and ground-state structure of the perovskite monolayers and bilayers, thus providing an important indicator for screening this hybrid improper ferroelectricity. Generally, the ferroelectric switching via an orthorho…
We present a systematic investigation of the role and importance of excitonic effects on the optical properties of transitions metal oxide perovskites. A representative set of fourteen compounds has been selected, including 3$d$ (SrTiO$_3$, LaScO$_3$, LaTiO$_3$, LaVO$_3$, LaCrO$_3$, LaMnO$_3$, LaFeO$_3$ and SrMnO$_3$), 4$d$ (SrZrO$_3$, SrTcO$_3$ and Ca$_2$RuO$_4$) and 5$d$ (SrHfO$_3$, KTaO$_3$ and NaOsO$_3$) perovskites, covering a band gap ranging from 0.1 eV to 6.1 eV and exhibiting different electronic, structural and magnetic properties. Optical conductivities and optical transitions inclu…
The many surface reconstructions of (110)-oriented lanthanum--strontium manganite (La$_{0.8}$Sr$_{0.2}$MnO$_3$, LSMO) were followed as a function of the oxygen chemical potential ($μ_\text{O}$) and the surface cation composition. Decreasing $μ_\text{O}$ causes Mn to migrate across the surface, enforcing phase separation into A-site-rich areas and a variety of composition-related, structurally diverse B-site-rich reconstructions. The composition of these phase-separated structures was quantified with scanning tunneling microscopy (STM), and these results were used to build a 2D phase diagram of…
Owing to the versatility in their chemical and physical properties, transition metal perovskite oxides have emerged as a new category of highly efficient photocatalysts for photoelectrochemical water splitting. Here, to understand the underlying mechanism for the enhanced photoelectrochemical water splitting in mixed perovskites, we explore ideal epitaxial thin films of the BiFeO3-SrTiO3 system. The electronic struture and carrier dynamics are determined from both experiment and density-functional theory calculations. The intrinsic phenomena are measured in this ideal sytem, contrasting to com…
