We have investigated the effects of structure change and electron correlation on SrTiO$_{3}$ single crystals using angle-resolved photoemission spectroscopy. We show that the cubic to tetragonal phase transition at 105$^\circ$K is manifested by a charge transfer from in-plane ($d_{yz}$ and $d_{zx}$) bands to out-of-plane ($d_{xy}$) band, which is opposite to the theoretical predictions. Along this second-order phase transition, we find a smooth evolution of the quasiparticle strength and effective masses. The in-plane band exhibits a peak-dip-hump lineshape, indicating a high degree of correlation on a relatively large (170 meV) energy scale, which is attributed to the polaron formation.
We investigated the magnetic and optical properties of [(LaMnO3)n/(SrTiO3)8]20 (n = 1, 2, and 8) superlattices grown by pulsed laser deposition. We found a weak ferromagnetic and semiconducting state developed in all superlattices. An analysis of the optical conductivity showed that the LaMnO3 layers in the superlattices were slightly doped. The amount of doping was almost identical regardless of the LaMnO3 layer thickness up to eight unit cells, suggesting that the effect is not limited to the interface. On the other hand, the magnetic ordering became less stable as the LaMnO3 layer thickness…
The possible existence of short-channel effects in oxide field-effect transistors is investigated by exploring field-effect transistors with various gate lengths fabricated from LaAlO$_3$-SrTiO$_3$ heterostructures. The studies reveal the existence of channel-length modulation and drain-induced barrier lowering for gate lengths below 1 μm, with a characteristic behavior comparable to semiconducting devices. With the fabrication of field-effect transistors with gate lengths as small as 60 nm the results demonstrate the possibility to fabricate by electron-beam lithography functional devices bas…
Oxygen vacancies are an important type of defect in transition metal oxides. In SrTiO$_3$ they are believed to be the main donors in an otherwise intrinsic crystal. At the same time, a relatively deep gap state associated with the vacancy is widely reported. To explain this inconsistency we investigate the effect of electron correlation in an oxygen vacancy (OV) in SrTiO$_3$. When taking correlation into account, we find that the OV-induced localized level can at most trap one electron, while the second electron occupies the conduction band. Our results offer a natural explanation of how the O…
We shed light on the interplay between structure and many-body effects relevant for itinerant ferromagnetism in LaAlO$_3$/SrTiO$_3$ heterostructures. The realistic correlated electronic structure is studied by means of the (spin-polarized) charge self-consistent combination of density functional theory (DFT) with dynamical mean-field theory (DMFT) beyond the realm of static correlation effects. Though many-body behavior is also active in the defect-free interface, a ferromagnetic instability occurs only with oxygen vacancies. A minimal Ti two-orbital $e_g$-$t_{2g}$ description for the correlat…
Motivated by the puzzling report of the observation of a ferromagnetic insulating state in LaMnO$_3$/SrTiO$_3$ heterostructures, we calculate the electronic and magnetic state of LaMnO$_3$, coherently matched to a SrTiO$_3$ square substrate within a "strained-bulk" geometry. We employ three different density functional theory based computational approaches: (a) density functional theory (DFT) supplemented with Hubbard U (DFT+U), (b) DFT + dynamical mean field theory (DMFT), and (c) a hybrid functional treatment of the exchange-correlation functional. While the first two approaches include loca…
The electrical and structural characteristics of SmTiO3/SrTiO3/SmTiO3 and GdTiO3/SrTiO3/GdTiO3 heterostructures are compared. Both types of structures contain narrow SrTiO3 quantum wells, which accommodate a confined, high-density electron gas. As shown previously [Phys. Rev. B 86, 201102(R) (2012)] SrTiO3 quantum wells embedded in GdTiO3 show a metal-to-insulator transition when their thickness is reduced so that they contain only two SrO layers. In contrast, quantum wells embedded in SmTiO3 remain metallic down to a single SrO layer thickness. Symmetry-lowering structural distortions, measur…
In this paper, we report the applicability of the density matrix renormalization group(DMRG) approach to the cylindrical single wall carbon nanotube (SWCN) for purpose of its correlation effect. By applying the DMRG approach to the $t$+$U$+$V$ model, with $t$ and $V$ being the hopping and Coulomb energies between the nearest neighboring sites, respectively, and $U$ the onsite Coulomb energy, we calculate the phase diagram for the SWCN with chiral numbers ($n_{1}=3, n_{2}=2$), which reflects the competition between the correlation energy $U$ and $V$. Within reasonable parameter ranges, we inves…
We present x-ray reflectivity, x-ray diffraction and atomic force microscopy measurements of single crystal SrTiO3 taken as a function of temperature. We found a rumpling transformation of the SrTiO3 surface after cooling the sample below ~105 K. The rumpling transformation is correlated with the cubic to tetragonal phase transformation that occurs at the same temperature. The rumpling transformation is reversible.
The use of SrTiO$_3$ dielectrics as high-permittivity insulator in organic thin film field effect transistors (FET) is evaluated. Field-effect transistors with sputtered SrTiO$_3$ and copper-phthalocyanine (CuPc) as semiconducting layer were fabricated. The device preparation was performed in-situ in an ultra high vacuum chamber system. The dielectric in the transistors had a permittivity of up to 200 which led to low driving voltages of 3 V. The field effect transistors were p-type and reached mobilities of about $μ= 1.5\times 10^{-3}$ cm$^2$/Vs and an on/off ratio of $10^3$. These properties…
By combined top- and backgating, we explore the correlation of superconductivity with band filling and electron confinement at the LaAlO$_3$-SrTiO$_3$ interface. We find that the top- and backgate voltages have distinctly different effects on the superconducting critical temperature, implying that the confining potential well has a profound effect on superconductivity. We investigate the origin of this behavior by comparing the gate-dependence of $T_c$ to the corresponding evolution of the band filling with gate voltage. For several backgate voltages, we observe maximum $T_c$ to consistently c…
We found that a surface state induced by hydrogenation on the surface of SrTiO$_{3}$(001) (STO) did not obey the rigid band model, which was confirmed by in situ electrical resistivity measurements in ultrahigh vacuum. With exposure of atomic hydrogen on the STO, a new surface state (H-induced donor state, HDS) appears within the bulk band gap (an in-gap state), which donates electrons thermally activated to the bulk conduction band, resulting in downward bending of the bulk bands beneath the surface. The doped electrons flow through the space-charge layer in two-dimensional manner parallel to…
The origin of the $3 \times 1$ reconstruction observed in epitaxial LaCoO$_{3}$ films on SrTiO$_3(001)$ is assessed by using first-principles calculations including a Coulomb repulsion term. We compile a phase diagram as a function of the oxygen pressure, which shows that ($3 \times 1$)-ordered oxygen vacancies (LaCoO$_{2.67}$) are favored under commonly used growth conditions, while stoichiometric films emerge under oxygen-rich conditions. Growth of further reduced LaCoO$_{2.5}$ brownmillerite films is impeded by phase separation. We report two competing ground-state candidates for stoichiome…
The emerging material class of complex-oxides, where manipulation of physical properties lead to new functionalities at their heterointerfaces, is expected to open new frontiers in Spintronics. For example, SrRuO_3 is a promising material where external stimuli like strain, temperature and structural distortions control the stability of electronic and magnetic states, across its magnetic phase transition, useful for Spintronics. Despite this, not much has been studied to understand such correlations in SrRuO_3. Here we explore the influence of electron-lattice correlation to electron-transport…
The role of electronic correlation effects for a realistic description of the electronic properties of LaAlO3/SrTiO3 heterostructures as covered by the on-site Coulomb repulsion within the GGA+U approach is investigated. Performing a systematic variation of the values of the Coulomb parameters applied to the Ti 3d and La 4f orbitals we put previous suggestions to include a large value for the La 4f states into perspective. Furthermore, our calculations provide deeper insight into the band gap landscape in the space spanned by these Coulomb parameters and the resulting complex interference effe…
SrTiO$_3$ is a model perovskite compound with unique properties and technological relevance. At 105 K it undergoes a transition from a cubic to a tetragonal phase with characteristic antiferrodistortive rotations of the TiO$_6$ octahedra. Here we study systematically the effect of different exchange correlation functionals on the structural, electronic and optical properties of cubic and tetragonal STO by comparing the recently implemented strongly constrained and appropriately normed (SCAN) meta-GGA functional with the generalized gradient approximation (PBE96 and PBEsol) and the hybrid funct…
Intrinsic, two-dimensional ferromagnetic semiconductors are an important class of materials for overcoming the limitations of dilute magnetic semiconductors for spintronics applications. CrSiTe$_3$ is a particularly interesting member of this class, since it can likely be exfoliated down to single layers, where T$_C$ is predicted to increase dramatically. Establishing the nature of the magnetism in the bulk is a necessary precursor to understanding the magnetic behavior in thin film samples and the possible applications of this material. In this work, we use elastic and inelastic neutron scatt…
By pulsed-laser deposition epitaxial thin films of Sr_2FeMoO_6 have been pre- pared on (100) SrTiO_3 substrates. Already for a deposition temperature of 320 C epitaxial growth is achieved. Depending on deposition parameters the films show metallic or semiconducting behavior. At high (low) deposition temperature the Fe,Mo sublattice has a rock-salt (random) structure. The metallic samples have a large negative magnetoresistance which peaks at the Curie temperature. The magnetic moment was determined to 4 mu_B per formula unit (f.u.), in agreement with the expected value for an ideal ferrimagnet…
Quantum confinement at complex oxide interfaces establishes an intricate hierarchy of the strongly correlated $d$-orbitals which is widely recognized as a source of emergent physics. The most prominent example is the (001) LaAlO$_3$/SrTiO$_3$(LAO/STO) interface, which features a dome-shaped phase diagram of superconducting critical temperature and spin-orbit coupling (SOC) as a function of electrostatic doping, arising from a selective occupancy of $t_{2g}$ orbitals of different character. Here we study (111)-oriented LAO/STO interfaces - where the three $t_{2g}$ orbitals contribute equally to…
In a common paradigm, the electronic structure of condensed matter is divided into weakly and strongly correlated compounds. While conventional band theory usually works well for the former class, many-body effects are essential for the latter. Materials like the familiar SrTiO$_3$ compound that bridge or even abandon this characterization scheme are highly interesting. Here it is shown by means of combining density functional theory with dynamical-mean field theory that oxygen vacancies on the STO (001) surface give rise to a dichotomy of weakly-correlated $t_{2g}$ low-energy quasiparticles a…
The 2-dimensional electron system at the interface between LaAlO$_{3}$ and SrTiO$_{3}$ has several unique properties that can be tuned by an externally applied gate voltage. In this work, we show that this gate-tunability extends to the effective band structure of the system. We combine a magnetotransport study on top-gated Hall bars with self-consistent Schrödinger-Poisson calculations and observe a Lifshitz transition at a density of $2.9\times10^{13}$ cm$^{-2}$. Above the transition, the carrier density of one of the conducting bands decreases with increasing gate voltage. This surprising d…
The interface between the polar LaAlO$_3$ and nonpolar SrTiO$_3$ layers has been shown to exhibit various electronic and magnetic phases such as two dimensional electron gas, superconductivity, magnetism and electronic phase separation. These rich phases are expected due to the strong interplay between charge, spin and orbital degree of freedom at the interface between these complex oxides, leading to the electronic reconstruction in this system. However, until now all of these new properties have been studied extensively based on the interfaces which involve a polar LaAlO$_3$ layer. To invest…
We show that the Bloch states in the conduction band of SrTiO$_3$ arise from the interplay between highly anisotropic hopping in sub-bands derived from the Ti $t_{2g}$ orbitals and spin-orbit coupling that mixes these orbitals. Because of the nearly flat-band characteristics for one of the principal axes, at sufficiently high doping these Bloch states become unstable with respect to electron interactions, resulting in Mott-like singlet correlations. These findings may be relevant to the anomalous electronic properties of SrTiO$_3$, including its unusual superconductivity.
Epitaxial La2NiMnO6 thin films have been grown on (001)-oriented SrTiO3 using the PLD technique. The thin films are semiconducting and FM with a TC close to 270K, a coercive field of 920Oe, and a saturation magnetization of 5muB per f.u. TEM, conducted at RT, reveals a majority phase having "I-centered" structure with a=c=1.4asub and b=2asub along with a minority phase-domains having "P-type" structure (asub being the lattice parameter of the perovskite structure). A discusion on the presence of Ni/Mn long-range ordering, in light of recent literature on double perovskites La2NiMnO6 is present…
First-principles prediction of energy band gaps in 18-valence electron semiconducting half-Heusler compounds: Exploring the role of exchange and correlation
We study the emergence of Berezinskii-Kosterlitz-Thouless (BKT) phases in (PbTiO$_3$)$_3$/(SrTiO$_3$)$_3$ superlattices by means of second-principles simulations. Beyond a threshold tensile epitaxial strain of $ε= 0.25 \%$ the local dipole moments within the superlattices are confined to the film-plane, and thus the polarization can be effectively considered as two-dimensional. The analysis of the decay of the dipole-dipole correlation with the distance, together with the study of the density of defects and its distribution as function of temperature, supports the existence of a BKT phase in a…
Electronic correlations are crucial to the low energy physics of metallic systems with localized $d$ and $f$ states; however, their effect on band insulators and semiconductors is typically negligible. Here, we measure the electronic structure of the half-Heusler compound FeVSb, a band insulator with filled shell configuration of 18 valence electrons per formula unit ($s^2 p^6 d^{10}$). Angle-resolved photoemission spectroscopy (ARPES) reveals a mass renormalization of $m^{*}/m_{bare}= 1.4$, where $m^{*}$ is the measured effective mass and $m_{bare}$ is the mass from density functional theory …
Emergent phases in the two-dimensional electron gas (2DEG) formed at the interface between two insulating oxides have attracted great attention in the past decade. We present ab-initio electronic structure calculations for the interface between a Mott insulator GdTiO$_3$ (GTO) and a band insulator SrTiO$_3$ (STO) and compare our results with those for the widely studied LaAlO$_3$/SrTiO$_3$ (LAO/STO) interface between two band insulators. Our GTO/STO results are in excellent agreement with experiments, but qualitatively different from LAO/STO. We find an interface carrier density of 0.5$e^{-}$/…
Using Coulomb correlation parameters appropriate for $π$-conjugated polymers (PCPs), and a nearest neighbor hopping integral that is arrived at by fitting the energy spectra of three zigzag semiconducting single-walled carbon nanotubes (S-SWCNTs), we are able to determine quantitatively the exciton energies and exciton binding energies of 29 S-SWCNTs within a semiempirical $π$-electron Hamiltonian that has been widely used for PCPs. Our work establishes the existence of a deep and fundamental relationship between PCPs and S-SWCNTs.
The band gap of SrTiO$_{3}$ retards its photocatalytic application. Regardless narrowing the band gap of the anion doped SrTiO$_{3}$, the anion doping structures have low photoconversion efficiency. The co-cation dopings are used to modify the band gap and band edges positions of SrTiO$_{3}$ to enhance the photocatalyitic properties by extending the absorption to longer visible-light. Using density functional calculations with the Heyd-Scuseria-Ernzerhof (HSE06) hybrid functional for exchange-correlation, the crystal and electronic structures as well as the optical properties of the mono and c…
High-quality thermoelectric LaxSr1-xTiO3 (LSTO) layers (here with x = 0.2), with thicknesses ranging from 20 nm to 700 nm, have been epitaxially grown on SrTiO3(001) substrates by enhanced solid-source oxide molecular-beam epitaxy. All films are atomically flat (with rms roughness < 0.2 nm), with low mosaicity (<0.1°), and present very low electrical resistivity (<5 x 10-4 ohm.cm at room temperature), one order of magnitude lower than commercial Nb-doped SrTiO3 single-crystalline substrate. The conservation of transport properties within this thickness range has been confirmed by thermoelectri…
Recently, monolayer CoSb/SrTiO$_3$ has been proposed as a candidate harboring interfacial superconductivity in analogy with monolayer FeSe/SrTiO$_3$. Experimentally, while the CoSb-based compounds manifesting as nanowires and thin films have been realized on SrTiO$_3$ substrates, serving as a rich playground, their electronic structures are still unknown and yet to be resolved. Here, we have fabricated CoSb$_{1-x}$ nanoribbons with quasi-one-dimensional stripes on SrTiO$_3$(001) substrates using molecular beam epitaxy, and investigated the electronic structure by in situ angle-resolved photoem…
Ultrafast terahertz spectroscopy accesses the {\em dark} excitonic ground state in resonantly-excited (6,5) SWNTs via internal, direct dipole-allowed transitions between lowest lying dark-bright pair state $\sim$6 meV. An analytical model reproduces the response which enables quantitative analysis of transient densities of dark excitons and {\em e-h} plasma, oscillator strength, transition energy renormalization and dynamics. %excitation-induced renormalization. Non-equilibrium, yet stable, quasi-1D quantum states with dark excitonic correlations rapidly emerge even with increasing off-resonan…
Silicon undergoes a phase transition from the semiconducting diamond phase to the metallic beta-Sn phase under pressure. We use quantum Monte Carlo calculations to predict the transformation pressure and compare the results to density functional calculations employing the LDA, PBE, PW91, WC, AM05, PBEsol and HSE06 exchange-correlation functionals. Diffusion Monte Carlo predicts a transition pressure of 14.0 +- 1.0 GPa slightly above the experimentally observed transition pressure range of 11.3 to 12.6 GPa. The HSE06 hybrid functional predicts a transition pressure of 12.4 GPa in excellent agre…
The electronic structure of the VAs compound in the zinc-blende structure is investigated using a combined density-functional and dynamical mean-field theory approach. Contrary to predictions of a ferromagnetic semiconducting ground state obtained by density-functional calculations, dynamical correlations induce a closing of the gap and produce a half-metallic ferromagnetic state. These results emphasize the importance of dynamic correlations in materials suitable for spintronics.
Organic materials have attracted recent interest as thermoelectric (TE) converters due to their low cost and ease of fabrication. We examine the effects of disorder on the TE properties of semiconducting polymers based on the Gaussian disorder model (GDM) for site energies while employing Pauli's master equation approach to model hopping between localized sites. Our model is in good agreement with experimental results and a useful tool to study hopping transport. We show that stronger overlap between sites can improve the electrical conductivity without adversely affecting the Seebeck coeffici…
The atomic, electronic structure and phonon frequencies have been calculated in a cubic and low-temperature tetragonal SrTiO3 phases at the ab initio level. We demonstrate that the use of hybrid exchange-correlation PBE0 functional gives the best agreement with experimental data. The results for the standard PBE and hybrid PBE0 are compared for the two types of basis sets: a linear combination of atomic orbitals (LCAO, CRYSTAL09 computer code) and plane waves (PW, VASP 5.2 code). Relation between cubic and tetragonal antiferrodistortive (AFD) phases and the relevant AFD phase transition observ…
Crystals of SrMn2Sb2 and BaMn2Sb2 were grown using Sn flux and characterized by powder and single-crystal x-ray diffraction, respectively, and by single-crystal electrical resistivity rho, heat capacity Cp, and magnetic susceptibility chi measurements versus temperature T, and magnetization versus field M(H) isotherm measurements. SrMn2Sb2 adopts the trigonal CaAl2Si2-type structure whereas BaMn2Sb2 crystallizes in the tetragonal ThCr2Si2-type structure. The rho(T) data indicate semiconducting behaviors for both compounds with activation energies of 0.35 eV for SrMn2Sb2 and 0.16 eV for BaMn2Sb…
To study digital Mott insulator LaTiO3 and band insulator SrTiO3 interfaces, we apply correlated band theory (LDA+U) to (n,m) multilayers, 1<n,m<9. If the on-site repulsion on Ti is large enough to model the magnetic insulating behavior of cubic bulk LaTiO3, the charge imbalance at the interface is found in all cases to be accommodated by disproportionation (Ti4+ + Ti3+), charge ordering, and Ti3+ d_xy-orbital ordering, with antiferromagnetic exchange coupling between the spins in the interface layer. Lattice relaxation affects the conduction behavior by shifting (slightly but importantly) the…
Key Role of Charge Disproportionation in Monoclinic Semiconducting Fe$_2$PO$_5$, a Room-Temperature d-Wave Altermagnet Candidate
Iowa State University（爱荷华州立大学）；South Dakota State University（南达科他州立大学）；University of Nebraska-Lincoln（内布拉斯加大学林肯分校）；Nebraska Center for Materials and Nanoscience（内布拉斯加材料与纳米科学中心）；Ames National Laboratory, U.S. Department of Energy（美国能源 Ames 国家实验室）
We investigate the physical properties and electronic structure of BaFe2-δSe3 crystals, which were grown out of tellurium flux. The crystal structure of the compound, an iron-deficient derivative of the ThCr2Si2-type, is built upon edge-shared FeSe4 tetrahedra fused into double chains. The semiconducting BaFe2-δSe3 with δ \approx 0.2 (ρ295K = 0.18 Ω\cdotcm and Eg = 0.30 eV) does not order magnetically, however there is evidence for short-range magnetic correlations of spin glass type (Tf \approx 50 K) in magnetization, heat capacity and neutron diffraction results. A one-third substitution of …
We report the electronic structure, electric and thermal transport properties of Ru$_{1-x}$Ir$_{x}$Se$_2$ ($x \leq 0.2$). RuSe$_2$ is a semiconductor that crystallizes in a cubic pyrite unit cell. The Seebeck coefficient of RuSe$_2$ exceeds -200 $μ$V/K around 730 K. Ir substitution results in the suppression of the resistivity and the Seebeck coefficient, suggesting the removal of the peaks in density of states near the Fermi level. Ru$_{0.8}$Ir$_{0.2}$Se$_{2}$ shows a semiconductor-metal crossover at about 30 K. The magnetic field restores the semiconducting behavior. Our results indicate the…
Superlattices composed of ferromagnetics, namely La$_{0.7}$Ca$_{0.3}$MnO$_3$ (LCMO), and ferroelectrics, namely, BaTiO$_3$(BTO) were grown on SrTiO$_3$ at 720$^o$C by pulsed laser deposition process. While the out-of-plane lattice parameters of the superlattices, as extracted from the X-ray diffraction studies, were found to be dependent on the BTO layer thickness, the in-plane lattice parameter is almost constant. The evolution of the strains, their nature, and their distribution in the samples, were examined by the conventional sin$^2ψ$ method. The effects of structural variation on the phys…
Dynamically suppressed lattice rotations in SrTiO$_3$ as a basis for photo-induced ferroelectricity
SLAC National Accelerator Laboratory（斯坦福直线加速器中心）；Max Planck Institute for the Structure and Dynamics of Matter（马克斯·普朗克物质结构与动力学研究所）；Cornell University（康奈尔大学）；Massachusetts Institute of Technology（麻省理工学院）；Arizona State University Biodesign Institute（亚利桑那州立大学生物设计研究院）；University of Oxford（牛津大学）
Quantitative Photoemission Predictions of Semiconducting Photocathodes from Many-Body Ab Initio Theory
Carl von Ossietzky Universität Oldenburg（奥尔登堡卡尔·冯·奥西茨基大学）；Friedrich-Schiller Universität Jena（耶拿弗里德里希·席勒大学）；Helmholtz-Zentrum Berlin（柏林赫尔姆霍兹中心）；Universität Siegen（锡根大学）；Humboldt-Universität zu Berlin（柏林洪堡大学）；Universitá degli Studi di Salerno（萨莱诺大学）
Previous first-principles calculations of the melting properties of Si, based on the local-density approximation (LDA) for electronic exchange-correlation energy, under-predict the melting temperature by ~ 20%. We present new first-principles results demonstrating that this problem is due to non-cancellation of exchange-correlation errors between the semiconducting solid and the metallic liquid. It is shown that other sources of error, particularly those due to system size and Brillouin-zone sampling, can be made negligible. The same LDA errors cause an underprediction of the pressure of the d…
