Effect of growth orientation on charge- and orbital-ordering (CO-OO) phenomena has been studied for Pr0.5Ca0.5MnO3 epitaxial thin films fabricated on (LaAlO3)0.3-(SrAl0.5Ta0.5O3)0.7 (LSAT) substrates by means of resistivity, synchrotron x-ray diffraction, and polarized optical microscopy measurements. CO-OO transition is observed around 220 K for a film grown on an LSAT (011) substrate ((011)-film), similarly to a bulk sample, while a film grown on a (001) plane of LSAT ((001)-film) shows much higher transition temperature around 300 K. The domain size of OO is approximately 3 times as large in the (011)-film as in the (001)-film. These results demonstrate that various properties of CO-OO phenomena can be controlled with the growth orientation via the epitaxial strain from the substrate.
We report the synthesis of Ca$_2$RuO$_4$ thin films on NdCaAlO$_{4}$ (110), LaAlO$_3$ (100) and LaSrAlO$_4$ (001) substrates and show that epitaxial strain induces a transition from the Mott-insulating phase of bulk Ca$_2$RuO$_4$ into a metallic phase. Magnetometry and spin-polarized neutron reflectometry reveal a low-temperature, small-moment ferromagnetic state in metallic Ca$_2$RuO$_4$ films.
We investigate in the framework of Landau theory the distortion of the strain fields at the interface of two dissimilar ferroelastic oxides that undergo a structural cubic-to-tetragonal phase transition. Simple analytical solutions are derived for the dilatational and the order parameter strains that are globally valid over the whole of the heterostructure. The solutions reveal that the dilatational strain exhibits compression close to the interface which may in turn affect the electronic properties in that region.
First-principles calculations reveal a large cooperative coupling of Jahn-Teller (JT) distortion to oxygen-octahedron rotations in perovskite LaMnO$_3$. The combination of the two distortions is responsible for stabilizing the strongly orthorhombic $A$-AFM insulating ($I$) $Pbnm$ ground state relative to a metallic ferromagnetic (FM-$M$) phase. However, epitaxial strain due to coherent matching to a crystalline substrate can change the relative stability of the two states. In particular, coherent matching to a square-lattice substrate favors the less orthorhombic FM-$M$ phase, with the $A$-AFM…
Perovskite nickelate heterostructure consisting of single unit cell of EuNiO$_3$ and LaNiO$_3$ have been grown on a set of single crystalline substrates by pulsed laser interval deposition to investigate the effect of epitaxial strain on electronic and magnetic properties at the extreme interface limit. Despite the variation of substrate in-plane lattice constants and lattice symmetry, the structural response to heterostructuring is primarily controlled by the presence of EuNiO$_3$ layer. In sharp contrast to bulk LaNiO$_3$ or EuNiO$_3$, the superlattices grown under tensile strains exhibit me…
High–quality epitaxial YNixMn1-xO3 thin films have been successfully grown on SrTiO3 (100) (STO) by pulsed laser deposition. X-ray diffraction studies showed that the films deposited on STO are fully c-axis oriented and exhibit in-plane alignment. The magnetic transition temperatures (Tc) of the films (both x=0.33 and 0.5) are equivalent to the values of the corresponding bulk samples. However, when x=0.5, the films show magnetic properties quite different from those of bulk samples. This difference may be caused by the structure distortion in these films.
The spin states of Co$^{3+}$ ions in perovskite-type LaCoO$_3$, governed by complex interplay between the electron-lattice interactions and the strong electron correlations, still remain controversial due to the lack of experimental techniques which can detect directly. In this letter, we revealed the tensile-strain dependence of spin states, $i. e.$ the ratio of the high- and low-spin states, in epitaxial thin films and a bulk crystal of LaCoO$_3$ via resonant inelastic soft x-ray scattering. The tensile-strain as small as 1.0% was found to realize different spin states from that in the bulk.
For an epitaxial Pr0.48Ca0.52MnO3 film on NdGaO3, we use transmission electron microscopy to observe a "charge-ordered" superlattice along the in-plane direction a. The same film shows no electrical signatures of charge order. The in-plane electrical anisotropy (rho)a/(rho)c = 28 is constant, and there is no evidence of sliding charge density waves up to the large field of ~10^3 V/cm.
Epitaxial thin films of LaCoO_{3} (E-LCO) exhibit ferromagnetic order with a transition temperature T_c = 85 K, while polycrystalline thin LaCoO_{3} films (P-LCO) remain paramagnetic. The temperature-dependent spin-state structure for both E-LCO and P-LCO was studied by x-ray absorption spectroscopy at the Co L_{2,3} and O K edges. Considerable spectral redistributions over temperature are observed for P-LCO. The spectra for E-LCO, on the other hand, do not show any significant changes for temperatures between 30 K and 450 K at both edges, indicating that the spin state remains constant and th…
We report on the synthesis of ultrathin films of highly distorted EuNiO3 (ENO) grown by interrupted pulse laser epitaxy on YAlO3 (YAO) substrates. Through mapping the phase space of nickelate thin film epitaxy, the optimal growth temperatures were found to scale linearly with the Goldschmidt tolerance factor. Considering the gibbs energy of the expanding film, this empirical trend is discussed in terms of epitaxial stabilization and the escalation of the lattice energy due to lattice distortions and decreasing symmetry. These findings are fundamental to other complex oxide perovskites, and pro…
The interrelation between the epitaxial strain and oxygen deficiency in La0.7Ca0.3MnO3-δ thin films was studied in terms of structural and functional properties. The films with a thickness of 1000Å were prepared using a PLD system equipped with a RHEED facility and a pyrometric film temperature control. The epitaxial strain and the oxygen deficiency in the samples were systematically modified using three different substrates: SrTiO3, (LaAlO3)0.3-(Sr2AlTaO6)0.7 and LaSrAlO4, and four different oxygen pressures during film growth ranging from 0.27mbar to 0.1mbar. It could be demonstrated that th…
We show that a ferromagnetic (FM) order in the orthorhombic CaRuO3, which is a non-magnetic and iso-structural analog of FM system SrRuO3, can be established and stabilized by the means of tensile epitaxial strain. Investigations on the structural and magnetic property correlations in the CaRuO3 films with different degrees of strain reveal that the FM moment increases with increasing the tensile strain. This is an experimental verification to the theoretical predictions of scaling of the tensile epitaxial strain and the magnetic order in this system. Our studies further establish that the ten…
We have synthesized epitaxial NdNiO$_{3}$ ultra-thin films in a layer-by-layer growth mode under tensile and compressive strain on SrTiO$_{3}$ (001) and LaAlO$_3$ (001), respectively. A combination of X-ray diffraction, temperature dependent resistivity, and soft X-ray absorption spectroscopy has been applied to elucidate electronic and structural properties of the samples. In contrast to the bulk NdNiO$_{3}$, the metal-insulator transition under compressive strain is found to be completely quenched, while the transition remains under the tensile strain albeit modified from the bulk behavior.
We have studied the influence of epitaxial strain on magnetic orderings and the couplings between the spin and polar phonons in the 1:1 SrMnO$_3$/LaMnO$_3$ superlattice from first principles. Magnetic phase transitions of the superlattice induced by epitaxial strain are observed, consistent with previous reports. We find that oxygen octahedral rotations lower the ground state energy but do not destroy the magnetic phase transitions induced by strain. We compute zone center phonon frequencies and eigenvectors as functions of epitaxial strain and magnetic ordering. A substantial increase of the …
We have studied structural and transport properties of epitaxial NaxCoO2 thin films on (0001) sapphire substrate prepared by topotaxially converting an epitaxial Co3O4 film to NaxCoO2 with annealing in Na vapor. The films are c axis oriented and in-plane aligned with [10 1 0] NaxCoO2 rotated by 30 degrees from [10 1 0] sapphire. Different Na vapor pressures during the annealing resulted in films with different Na concentrations, which showed distinct transport properties.
We report herein fabrication and characterization of a thin-film transistor (TFT) using single-crystalline, epitaxial SrTiO3 film, which was grown by a pulsed laser deposition technique followed by the thermal annealing treatment in an oxygen atmosphere. Although TFTs on the polycrystalline epitaxial SrTiO3 films (as-deposited) exhibited poor transistor characteristics, the annealed single-crystalline SrTiO3 TFT exhibits transistor characteristics comparable with those of bulk single-crystal SrTiO3 FET: an on/off current ratio >10^5, sub-threshold swing ~2.1 V/decade, and field-effect mobility…
Huge deformations of the crystal lattice can be achieved in materials with inherent structural instability by epitaxial straining. By coherent growth on seven different substrates the in-plane lattice constants of 50 nm thick Fe70Pd30 films are continuously varied. The maximum epitaxial strain reaches 8,3 % relative to the fcc lattice. The in-plane lattice strain results in a remarkable tetragonal distortion ranging from c/abct = 1.09 to 1.39, covering most of the Bain transformation path from fcc to bcc crystal structure. This has dramatic consequences for the magnetic key properties. Magneto…
First-principles density-functional calculations reveal a large spin-phonon coupling in cubic SrMnO$_{3}$, with ferromagnetic ordering producing a polar instability. Through combination of this coupling with the strain-polarization coupling characteristic of perovskites, the bulk antiferromagnetic paraelectric ground state of SrMnO$_3$ is shown to be driven to a previously unreported multiferroic ferroelectric-ferromagnetic state by increasing epitaxial strain, both tensile and compressive. This state has a computed polarization and estimated Curie temperature above 54 $μ$C/cm$^2$ and 92 K. La…
Multiferroics with the coexistence of ferroelectric and ferromagnetic orders are ideal candidates for magnetoelectric applications. Unfortunately, only very few ferroelectric-ferromagnetic multiferroics (with low magnetic critical temperature) were discovered. Here we perform first principles calculations to investigate the effects of the epitaxial strain on the properties of BiMnO3 films grown along the pseudocubic [001] direction. Unlike the ground state with the centrosymmetric C2/c space group in bulk, we reveal that the tensile epitaxial strain stabilizes the ferromagnetic and ferroelectr…
Perovskite LaTiO$_3$ bulk is a typical Mott-insulator with G-type antiferromagnetic order. In this work, the biaxial strain effects on the ground magnetic order of LaTiO$_3$ films grown on various substrates have been studied. For the compressive strain, LaTiO$_3$ films grown on LaAlO$_3$, LaGaO$_3$, and SrTiO$_3$ substrates undergo a phase transition from the original G-type antiferromagnet to A-type antiferromagnet. The underlying physical mechanisms are the lattice distortions tunned by strain. While for the tensile strain, the BaTiO$_3$ and LaScO$_3$ substrates have been tested, which show…
Multiferroic BiFeO3 epitaxial films with thickness ranging from 40 nm to 960 nm were grown by pulsed laser deposition on SrTiO3 (001) substrates with SrRuO3 bottom electrodes. X-ray characterization shows that the structure evolves from angularly-distorted tetragonal with c/a ~ 1.04 to more bulk-like distorted rhombohedral (c/a ~ 1.01) as the strain relaxes with increasing thickness. Despite this significant structural evolution, the ferroelectric polarization along the body diagonal of the distorted pseudo-cubic unit cells, as calculated from measurements along the normal direction, barely ch…
Ferromagnetic insulators play a crucial role in the development of low-dissipation quantum magnetic devices for spintronics. Epitaxial LaCoO3 thin film is a prominent ferromagnetic insulator, in which the robust ferromagnetic ordering emerges owing to epitaxial strain. Whereas it is evident that strong spin-lattice coupling induces ferromagnetism, the reported ferromagnetic properties of epitaxially strained LaCoO3 thin films were highly consistent. For example, even under largely modulated degree of strain, the reported Curie temperatures of epitaxially strained LaCoO3 thin films lie within 8…
Using density-functional theory calculations, we investigate the magnetic as well as the dynamical properties of tetragonal SrRuO3 (SRO) under the influence of epitaxial strain. It is found that both the tensile and compressive strain in the xy-plane could induce the abrupt change in the magnetic moment of Ru atom. In particular, under the in-plane ~4% compressive strain, a ferromagnetic to nonmagnetic transition is induced. Whereas for the tensile strain larger than 3%, the Ru magnetic moment drops gradually with the increase of the strain, exhibiting a weak ferromagnetic state. We find that …
We investigate the effect of epitaxial strain on the Mott metal-insulator transition (MIT) in perovskite systems with d^1 and d^2 electron configuration of the transition metal (TM) cation. We first discuss the general trends expected from the changes in the crystal-field splitting and in the hopping parameters that are induced by epitaxial strain. We argue that the strain-induced crystal-field splitting generally favors the Mott-insulating state, whereas the strain-induced changes in the hopping parameters favor the metallic state under compressive strain and the insulating state under tensil…
Oxygen packaging in transition metal oxides determines the metal-oxygen hybridization and electronic occupation at metal orbitals. Strontium vanadate (SrVO$_3$), having a single electron in a $3d$ orbital, is thought to be the simplest example of strongly correlated metallic oxides. Here, we determine the effects of epitaxial strain on the electronic properties of SrVO$_3$ thin films, where the metal-oxide sublattice is corner-connected. Using x-ray absorption and x-ray linear dichroism at the V $L_{2,3}$ and O $K$-edges, it is observed that tensile or compressive epitaxial strain change the h…
The effect of epitaxial strain on the structural and electronic properties of LaVO_3 is investigated through density functional theory (DFT) and dynamical mean field theory (DMFT). Two different growth orientations of the crystal are considered, one preserving the bulk Pbnm space-group symmetry and another giving rise to a symmetry lowering to P2_1/m. In the nonmagnetic DFT structures, the two growth orientations are equally favored for all tensile strains considered here, as well as for compressive strains weaker than -3%. For stronger compressive strains, the P2_1/m orientation is favored an…
We report x-ray synchrotron experiments on epitaxial films of uranium, deposited on niobium and tungsten seed layers. Despite similar lattice parameters for these refractory metals, the uranium epitaxial arrangements are different and the strains propagated along the a-axis of the uranium layers are of opposite sign. At low temperatures these changes in epitaxy result in dramatic modifications to the behavior of the charge-density wave in uranium. The differences are explained with the current theory for the electron-phonon coupling in the uranium lattice. Our results emphasize the intriguing …
We report on the preparation and characterization of epitaxial thin films of the double-perovskite Sr$_2$CrWO$_6$ by Pulsed Laser Deposition (PLD). On substrates with low lattice mismatch like SrTiO$_3$, epitaxial Sr$_2$CrWO$_6$ films with high crystalline quality can be grown in a molecular layer-by-layer growth mode. Due to the similar ionic radii of Cr and W, these elements show no sublattice order. Nevertheless, the measured Curie temperature is well above 400 K. Due to the reducing growth atmosphere required for double perovskites, the SrTiO$_3$ substrate surface undergoes an insulator-me…
A detailed investigation of the magnetization processes in epitaxial MnSi thin film reveals the existence of elliptically distorted skyrmion strings that lie in the plane of the film. We provide proof that the uniaxial anisotropy stabilizes this state over extended regions of the magnetic phase diagram. Theoretical analysis of an observed cascade of first-order phase transitions is based on rig- orous numerical calculations of competing chiral modulations, which shows the existence of helicoids, elliptic skyrmions, and cone phases.
A reversible structural transition of an epitaxial La2/3Sr1/3MnO3 film deposited on the LaAlO3 substrate has been investigated by means of in situ high-resolution transmission electron microscopy (HREM) and electron diffraction, combined with image and diffraction calculations. We observe that the crystallographic symmetry of the film can be lowered via electron beam irradiation, leading to a rhombohedral-monoclinic transition. This transition can be attributed to the cooperating effect of the mismatch stress and the irradiation-induced thermal-stress.
We report a giant resistance drop induced by dc electrical currents in La0.67Ca0.33MnO3 epitaxial thin films. Resistance of the patterned thin films decreases exponentially with increasing current and a maximum drop shows at the temperature of resistance peak Tp. Variation of resistance with current densities can be scaled below and above Tp, respectively. This work can be useful for the future applications of electroresistance.
We have studied electrical transport and magnetic properties of epitaxial La_0.66 Sr_0.33 Mn O_3 thin films grown on different substrates having different lattice strains induced by different film-substrate lattice-mismatch. Both electrical transport and magnetic properties exhibit strong correlation with Jahn-Teller strain. Our study shows a sufficiently large Jahn-Teller strain giving rise to distinct semi-conducting/insulating state in LSMO thin films even below the respective para-ferromagnetic Curie temperatutes Tc, which is in contradiction with the established phase diagram of Sr-doped …
Using {\it ab initio} methods, we investigate the modification of the magnetic properties of the $m=2$ member of the strontium iridates Ruddlesden-Popper series Sr$_{m+1}$Ir$_{m}$O$_{3m+1}$, bilayer Sr$_3$Ir$_2$O$_7$, induced by epitaxial strain and oxygen vacancies. Unlike the single layer compound Sr$_2$IrO$_4$, which exhibits a robust in-plane magnetic order, the energy difference between in-plane and out-of-plane magnetic orderings in Sr$_3$Ir$_2$O$_7$ is much smaller and it is expected that small external perturbations could induce magnetic transitions. Our results indicate that epitaxial…
We have synthesized epitaxial Sr2IrO4 thin-films on various substrates and studied their electronic structures as a function of lattice-strains. Under tensile (compressive) strains, increased (decreased) Ir-O-Ir bond-angles are expected to result in increased (decreased) electronic bandwidths. However, we have observed that the two optical absorption peaks near 0.5 eV and 1.0 eV are shifted to higher (lower) energies under tensile (compressive) strains, indicating that the electronic-correlation energy is also affected by in-plane lattice-strains. The effective tuning of electronic structures …
The impact of epitaxial strain on the structural, electronic, and thermoelectric properties of p-type transparent Sr-doped LaCrO3 thin films has been investigated. For this purpose, high-quality fully strained La0.75Sr0.25CrO3 (LSCO) epitaxial thin films were grown by molecular beam epitaxy on three different (pseudo)cubic (001)-oriented perovskite oxide substrates: LaAlO3, (LaAlO3)0.3(Sr2AlTaO6)0.7, and DyScO3. The lattice mismatch between the LSCO films and the substrates induces in-plane strain ranging from -2.06% (compressive) to +1.75% (tensile). The electric conductivity can be controlle…
Magneto-transport properties have been investigated for epitaxial thin films of B20-type MnSi grown on Si(111) substrates. Both Lorentz transmission electron microscopy (TEM) images and topological Hall effect (THE) clearly point to the robust formation of skyrmions over a wide temperature-magnetic field region. New features distinct from those of bulk MnSi are observed for epitaxial MnSi films: a shorter (nearly half) period of the spin helix and skyrmions, and an opposite sign of THE. These observations suggest versatile features of skyrmion-induced THE beyond the current understanding.
The discovery of high temperature superconductivity in FeSe films on SrTiO3 substrate has inspired great experimental and theoretical interests. First-principles density functional theory calculations, which have played an important role in the study of bulk iron-based superconductors, also participate in the investigation of interfacial superconductivity. In this article, we review the calculation results on the electronic and magnetic structures of FeSe epitaxial films, emphasizing on the interplay between different degrees of freedom, such as charge, spin, and lattice vibrations. Furthermor…
We have synthesized thermodynamically metastable Ca2IrO4 thin-films on YAlO3 (110) substrates by pulsed laser deposition. The epitaxial Ca2IrO4 thin-films are of K2NiF4-type tetragonal structure. Transport and optical spectroscopy measurements indicate that the electronic structure of the Ca2IrO4 thin-films is similar to that of Jeff = 1/2 spin-orbit-coupled Mott insulator Sr2IrO4 and Ba2IrO4, with the exception of an increased gap energy. The gap increase is to be expected in Ca2IrO4 due to its increased octahedral rotation and tilting, which results in enhanced electron-correlation, U/W. Our…
We have investigated the transport and optical properties along the c-axis of a-axis-oriented Sr2IrO4 epitaxial thin-films grown on LaSrGaO4 (100) substrates. The c-axis resistivity is approximately one order of magnitude larger than that of the ab-plane. Optical absorption spectra with E//b polarization show both Ir 5d intersite transitions and charge-transfer transitions (O 2p to Ir 5d), while E//c spectra show only the latter. The structural anisotropy created by biaxial strain in a-axis-oriented thin-films also changes the electronic structure and gap energy. These a-axis-oriented, epitaxi…
We have synthesized epitaxial Ba2IrO4 (BIO) thin-films on SrTiO3 (001) substrates by pulsed laser deposition and studied their electronic structure by dc-transport and optical spectroscopic experiments. We have observed that BIO thin-films are insulating but close to the metalinsulator transition boundary with significantly smaller transport and optical gap energies than its sister compound, Sr2IrO4. Moreover, BIO thin-films have both an enhanced electronic bandwidth and electronic-correlation energy. Our results suggest that BIO thin-films have great potential for realizing the interesting ph…
