Control of thin film stoichiometry is of primary relevance to achieve desired functionality. Pulsed laser deposition ablating from binary-oxide targets (sequential deposition) can be applied to precisely control the film composition, offsetting the importance of growth conditions on the film stoichiometry. In this work, we demonstrate that the cation stoichiometry of SrTiO$_3$ thin films can be finely tuned by sequential deposition from SrO and TiO$_2$ targets. Homoepitaxial SrTiO$_3$ films were deposited at different substrate temperatures and Ti/Sr pulse ratios, allowing the establishment of a growth window for stoichiometric SrTiO$_3$. The growth kinetics and nucleation processes were studied by reflection high-energy electron diffraction and atomic force microscopy, providing information about the growth mode and the degree of off-stoichiometry. At the optimal (stoichiometric) growth conditions, films exhibit atomically flat surfaces, whereas off-stoichiometry is accommodated by crystal defects, 3D islands and/or surface precipitates depending on the substrate temperature and the excess cation. This technique opens the way to precisely control stoichiometry and doping of oxide thin films.
The properties of single-crystal SrTiO$_{3}$ substrates and homoepitaxial SrTiO$_{3}$ films grown by pulsed laser deposition have been compared, in order to understand the loss of interfacial conductivity when more than a critical thickness of nominally homoepitaxial SrTiO$_{3}$ is inserted between a LaAlO$_{3}$ film and a SrTiO$_{3}$ substrate. In particular, the chemical composition and the structure of homoepitaxial SrTiO$_{3}$ investigated by low-energy ion-scattering and surface x-ray diffraction, show that for insulating heterointerfaces, a Sr-excess is present between the LaAlO$_{3}$ an…
The initial homoepitaxial growth of SrTiO3 on a (\surd13\times\surd13) - R33.7°SrTiO3(001) substrate surface, which can be prepared under oxide growth conditions, is atomically resolved by scanning tunneling microscopy. The identical (\surd13\times\surd13) atomic structure is clearly visualized on the deposited SrTiO3 film surface as well as on the substrate. This result indicates the transfer of the topmost Ti-rich (\surd13\times\surd13) structure to the film surface and atomic-scale coherent epitaxy at the film/substrate interface. Such atomically ordered SrTiO3 substrates can be applied to …
We have investigated the atomically-resolved substrate and homoepitaxial thin film surfaces of SrTiO3(001) using low-temperature scanning tunneling microscopy/spectroscopy (STM/STS) combined with pulsed laser deposition (PLD). It was found that annealing at 1000 oC in an oxygen partial pressure of 1*10-6 Torr, which is a typical annealing treatment for the preparation of SrTiO3 substrates, unexpectedly resulted in a disordered surface on an atomic scale. In contrast, homoepitaxial SrTiO3 thin films grown on this disordered substrate exhibited (2*2) surface reconstructions. The differential con…
Pulsed Laser Deposition (PLD) is widely used to grow epitaxial thin films of quantum materials such as complex oxides. Here, we use in-situ X-ray scattering to study homoepitaxy of SrTiO$_3$ by energetic (e-) and thermalized (th-) PLD. We find that e-PLD suppresses the lateral growth of two-dimensional islands, which suggests that energetic particles break up smaller islands. Fast interlayer transport occurs for both e-PLD and th-PLD, implying a process operating on sub-microsecond timescales that doesn't depend strongly on the kinetic energy of the incident particles.
In many transition metal oxides (TMOs), oxygen stoichiometry is one of the most critical parameters that plays a key role in determining the structural, physical, optical, and electrochemical properties of the material. However, controlling the growth to obtain high quality single crystal films having the right oxygen stoichiometry, especially in a high vacuum environment, has been viewed as a challenge. In this work, we show that through proper control of the plume kinetic energy, stoichiometric crystalline films can be synthesized without generating oxygen defects, even in high vacuum. We us…
The homoepitaxial growth of initially flat surfaces has so far always led to surfaces which become rougher and rougher as the number of layers increases: even in systems exhibiting ``layer by layer'' growth the registry of the layers is gradually lost. We propose that pulsed glancing-angle sputtering, once per monolayer, can in principle lead to layer-by-layer growth that continues indefinitely, if one additional parameter is controlled. We illustrate our suggestion with a fairly realistic simulation of the growth of a Pt (111) surface, coupled with a simplified model for the sputtering proces…
Pulsed laser deposition of SrTiO3/LaGaO3 and SrTiO3/LaAlO3 interfaces has been analyzed with a focus on the kinetic energy of the ablated species. LaGaO3 and LaAlO3 plasma plumes were studied by fast photography and space-resolved optical emission spectroscopy. Reflection high energy electron diffraction was performed proving a layer-by-layer growth up to 10-1 mbar oxygen pressure. The role of the energetic plasma plume on the two-dimensional growth and the presence of interfacial defects at different oxygen growth pressure has been discussed in view of the conducting properties developing at …
We discuss the origin of the temperature dependence of resistivity observed in highly oriented LaNiO_3 thin films (of thickness d) grown on SrTiO_3 substrate by a pulsed laser deposition technique. All the experimental data are found to collapse into a single universal curve [T/T_{sf}(d)]^{3/2} for the entire temperature interval (20K<T<300K) with T_{sf}(d) being the onset temperature for triggering a resonant scattering of conduction electrons by spin fluctuations in LaNiO_3/SrTiO_3 heterostructure.
We have studied the growth dynamics and electronic properties of SrTiO3-d homoepitaxial films by pulsed laser deposition. We find the two dominant factors determining the growth mode are the kinetics of surface crystallization and oxidation. When matched, persistent two-dimensional layer-by-layer growth can be obtained for hundreds of unit cells. By tuning these kinetic factors, oxygen vacancies can be frozen in the film, allowing controlled, systematic doping across a metal-insulator transition. Metallic films can be grown, exhibiting Hall mobilities as high as 25,000 cm2/Vs.
We have prepared the dilute magnetic semiconductor (DMS) InMnAs with different Mn concentrations by ion implantation and pulsed laser melting. The Curie temperature of the In1-xMnxAs epilayer depends on the Mn concentration x, reaching 82 K for x=0.105. The substitution of Mn ions at the Indium sites induces a compressive strain perpendicular to the InMnAs layer and a tensile strain along the in-plane direction. This gives rise to a large perpendicular magnetic anisotropy, which is often needed for the demonstration of electrical control of magnetization and for spin-transfer-torque induced ma…
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…
High quality epitaxial thin-films of EuTiO3 have been grown on the (001) surface of SrTiO3 using pulsed laser deposition. In situ x-ray reflectivity measurements reveal that the growth is two-dimensional and enable real-time monitoring of the film thickness and roughness during growth. The film thickness, surface mosaic, surface roughness, and strain were characterized in detail using ex situ x-ray diffraction. The thicnkess and composition were confirmed with Rutherford Backscattering. The EuTiO3 films grow two-dimensionally, epitaxially, pseudomorphically, with no measurable in-plane lattice…
Effect of biaxial tensile strains on optical functions and band edge transitions of ultra thin epitaxial films was studied using as an example a 13 nm thick SrTiO3 films deposited on KTaO3(100) single-crystal substrates. Optical functions were determined by spectroscopic ellipsometry technique. It was found that tensile strains result in a shift of the low energy band gap optical transitions to higher energies and decrease the refractive index in the visible region. Comparison of the optical spectra for strained SrTiO3 films and for homoepitaxial strain-free SrTiO3:Cr (0.01 %at.) films deposit…
The crystal structures of LaAlO3 films grown by pulsed laser deposition on SrTiO3 substrates at oxygen pressure of 10-3 mbar or 10-5 mbar, where kinetics of ablated species hardly depend on oxygen background pressure, are compared. Our results show that the interface between LaAlO3 and SrTiO3 is sharper when the oxygen pressure is lower. Over time, the formation of various crystalline phases is observed while the crystalline thickness of the LaAlO3 layer remains unchanged. X-ray scattering as well as atomic force microscopy measurements indicate three-dimensional growth of such phases, which a…
Pulsed Laser Deposition (PLD) of homoepitaxial SrTiO3 <001> was studied with in-situ x-ray specular reflectivity and surface diffuse x-ray scattering. Unlike prior reflectivity-based studies, these measurements access both the time- and the length-scales of the evolution of the surface morphology during growth. In particular, we show that this technique allows direct measurements of the diffusivity for both inter- and intra-layer transport. Our results explicitly limit the possible role of island break-up, demonstrate the key roles played by nucleation and coarsening in PLD, and place an upper…
High-mobility oxide heterostructures could be applied for high-frequency devices, transparent conductors, and spin-orbit logic devices. SrTiO$_3$ is one of the most studied oxide substrate materials for heterostructures. To date, the highest SrTiO3-based charge carrier mobility at 2 K was measured in the interfacial 2-dimensional electron gas (2DEG) of $γ$-Al$_2$O$_3$/SrTiO$_3$. The formation mechanism and origin of the high electron mobility are not yet fully understood. This investigation presents a successful growth protocol to synthesise high mobility $γ$-Al$_2$O$_3$/SrTiO$_3$ interfaces, …
Unlike widely explored complex oxide heterostructures grown along [001], the study of [111]-oriented heterointerfaces are very limited thus far. One of the main challenges is to overcome the polar discontinuity that hinders the epitaxy of atomically sharp interfaces. Here, by taking the LaCoO3/SrTiO3(111) as a prototype, we show that the reconstruction, which effectively compensates the surface polarity, can stabilize the epitaxy of the heterostructure with polar discontinuity. Reconstructed substrate surface is prepared, while the growth is controlled to form reconstruction on the film surfac…
Recently, Bi2O2Se is discovered as a promising two-dimensional (2D) semiconductor for next generation electronics, due to its moderate bandgap size, high electron mobility and pronounced ambient stability. Meanwhile, it has been predicted that high quality Bi2O2Se-related heterostructures may possess exotic physical phenomena, such as piezoelectricity and topological superconductivity. Herein, we report the first successful heteroepitaxial growth of Bi2O2Se films on SrTiO3 substrates via pulsed laser deposition (PLD) method. Films obtained under optimal conditions show an epitaxial growth with…
We have investigated the properties of interfaces between LaAlO3 films grown on SrTiO3 substrates singly terminated by TiO2. We used RF sputtering in a high-pressure oxygen atmosphere. The films are smooth, with flat surfaces. Transmission Electron Microscopy shows atomically sharp and continuous interfaces while EELS measurements show some slight intermixing. The elemental ratio of La to Al measured by EDX is found to be 1.07. Importantly, we find these interfaces to be non-conducting, indicating that the sputtered interface is not electronically reconstructed in the way reported for films gr…
The surface structure of SrTiO3(001) thin films homoepitaxially grown by PLD in step-flow mode was characterized using low temperature STM. It was found that one-dimensional (1D) TiOx-based nanostructures were formed on the thin film surface and their density increased with increasing thin film thickness. Most of the 1D nanostructures disappeared after a post-deposition annealing, indicating that this structure is metastable due to the nonequilibrium growth mode. The resulting surface after annealing exhibited similar features to that of a thinner film, having a domain structure with (2x1) and…
We present a comprehensive study of the thickness dependence of static and magneto-dynamic magnetic properties of La$_{0.7}$Sr$_{0.3}$MnO$_3$. Epitaxial pulsed laser deposited La$_{0.7}$Sr$_{0.3}$MnO$_3$ / SrTiO$_3$(001) thin films in the range from 3 unit cells (uc) to 40 uc (1.2 - 16 nm) have been investigated through ferromagnetic resonance spectroscopy (FMR) and SQUID magnetometry at variable temperature. Magnetodynamically, three different thickness, $d$, regimes are identified: 20 uc $\lesssim d$ uc where the system is bulk like, a transition region 8 uc $\le d \lesssim 20$ uc where the …
An experimental study was conducted on controlling the growth mode of La0.7Sr0.3MnO3 thin films on SrTiO3 substrates using pulsed laser deposition (PLD) by tuning growth temperature, pressure and laser fluence. Different thin film morphology, crystallinity and stoichiometry have been observed depending on growth parameters. To understand the microscopic origin, the adatom nucleation, step advance processes and their relationship to film growth were theoretically analyzed and a growth diagram was constructed. Three boundaries between highly and poorly crystallized growth, 2D and 3D growth, stoi…
Reflection high-energy electron diffraction (RHEED) is a ubiquitous in situ molecular beam epitaxial (MBE) characterization tool. Although RHEED can be a powerful means for crystal surface structure determination, it is often used as a static qualitative surface characterization method at discrete intervals during a growth. A full analysis of RHEED data collected during the entirety of MBE growths is made possible using principle component analysis (PCA) and k-means clustering to examine significant boundaries that occur in the temporal clusters grouped from RHEED data and identify statistical…
Growth of perovskite oxide thin films on Si in crystalline form has long been a critical obstacle for the integration of multifunctional oxides into Si-based technologies. In this study, we propose pulsed laser deposition of a crystalline SrTiO3 thin film on a Si using graphene substrate. The SrTiO3 thin film on graphene has a highly (00l)-oriented crystalline structure which results from the partial epitaxy. Moreover, graphene promotes a sharp interface by highly suppressing the chemical intermixing. The important role of graphene as a 2D substrate and diffusion barrier allows expansion of de…
Ferroelectric BiFeO3 thin films and artificial superlattices of (BiFeO3)m(SrTiO3)m (m~ 1 to 10 unit cells) were fabricated on (001)-oriented SrTiO3 substrates by pulsed laser ablation. The variation of leakage current and macroscopic polarization with periodicity was studied. Piezo force microscopy studies revealed the presence of large ferroelectric domains in the case of BiFeO3 thin films while a size reduction in ferroelectric domains was observed in the case of superlattice structures. The results show that the modification of ferroelectric domains through superlattice, could provide an ad…
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…
We investigate the effect of the laser parameters of pulsed laser deposition on the film stoichiometry and electronic properties of LaAlO_3/SrTiO_3 (001) heterostructures. The La/Al ratio in the LaAlO_3 films was varied over a wide range from 0.88 to 1.15, and was found to have a strong effect on the interface conductivity. In particular, the carrier density is modulated over more than two orders of magnitude. The film lattice expansion, caused by cation vacancies, is found to be the important functional parameter. These results can be understood to arise from the variations in the electrostat…
Nb-doped SrTiO$_{3}$ epitaxial thin films have been prepared on (001) SrTiO$_{3}$ substrates using pulsed laser deposition. A high substrate temperature ($>1000^{\circ}{C}$) was found to be necessary to achieve 2-dimensional growth. Atomic force microscopy reveals atomically flat surfaces with 3.9 Å$ $ steps. The films show a metallic behavior, residual resistivity ratios between 10 and 100, and low residual resistivity of the order of 10$^{-4}$$Ω$cm. At 0.3 K, a sharp superconducting transition, reaching zero resistance, is observed.
We combined photoelemission spectroscopy with first-principle calculations to investigate structural and electronic properties of SrTiO$_{3}$ doped with Ni impurities. In SrTiO$_{3}$ polycrystalline thin films, grown by magnetron sputtering, the mean size of the crystallites increases with the concentration of Ni. To determine the electronic band structure of SrTiO$_{3}$ films doped with Ni, high quality ordered pristine and SrTiO3:Ni$_{x}$ films with x=0.06 and 0.12 were prepared by pulsed laser deposition. Electronic band structure calculations for the ground state, as well as one-step model…
We report the observation that thermoelectric thin-films of La-doped SrTiO3 grown on SrTiO3 substrates yield anomalously high values of thermopower to give extraordinary values of power factor at 300K. Thin-films of Sr0.98La0.02TiO3, grown via pulsed laser deposition at low temperature and low pressure (450C, 10-7Torr), do not yield similarly high values when grown on other substrates. The thin-film growth induces oxygen reduction in the SrTiO3 crystals, doping the substrate n-type. It is found that the backside resistance of the SrTiO3 substrates is as low (~12ohm/square) as it is on the film…
LaAlO$_{3}$ and NdGaO$_{3}$ thin films of different thickness have been grown by pulsed laser deposition on TiO$_2$-terminated SrTiO$_{3}$ single crystals and investigated by soft X-ray photoemission spectroscopy. The surface sensitivity of the measurements has been tuned by varying photon energy $hν$ and emission angle $Θ$. In contrast to the core levels of the other elements, the Sr $3d$ line shows an unexpected splitting for higher surface sensitivity, signaling the presence of a second strontium component. From our quantitative analysis we conclude that during the growth process Sr atoms d…
SrTiO$_3$ is a promising $n$-type oxide semiconductor for thermoelectric energy conversion. Epitaxial thin films of SrTiO$_3$ doped with both La and oxygen vacancies have been synthesized by pulsed laser deposition (PLD). The thermoelectric and galvanomagnetic properties of these films have been characterized at temperatures ranging from 300 K to 900 K and are typical of a doped semiconductor. Thermopower values of double-doped films are comparable to previous studies of La doped single crystals at similar carrier concentrations. The highest thermoelectric figure of merit ($ZT$) was measured t…
We report the structural and transport properties of LaNiO3 thin films prepared by pulsed laser deposition technique. To understand the effects of film thickness, lattice mismatch and grain size on transport properties, various oriented substrates were used for deposition, including single-crystalline SrLaAlO4 (001), SrTiO3 (100) and LaAlO3 (100). To achieve a high quality LaNiO3 thin films, the vital parameters (such as laser fluence, substrate temperature, oxygen pressure, and deposition time) were optimized. The best quality films are found to be well textured samples with good crystalline …
Several SrTiO3 (STO) thin films without electrodes processed by pulsed laser deposition, of thicknesses down to 40 nm, were studied using infrared transmission and reflection spectroscopy. The complex dielectric responses of polar phonon modes, particularly ferroelectric soft mode, in the films were determined quantitatively. The compressed epitaxial STO films on (100) La0.18Sr0.82Al0.59-Ta0.41O3 substrates (strain 0.9%) show strongly stiffened phonon responses, whereas the soft mode in polycrystalline film on (0001) sapphire substrate shows a strong broadening due to grain boundaries and/or o…
In a recent work by Ji Seop Oh et al., BaBiO3(001) thin films were grown on SrTiO3 by Pulsed Laser Deposition. It was argued that the films are BiO2-terminated from the modelling of angle-resolved photoemission spectroscopy experiments. The authors claim, in opposition to previous theoretical predictions, that there are no metallic surface states on their films. In this short comment we question that the authors have enough evidence to make such a claim, as we consider that the large mismatch between SrTiO3 and BaBiO3 and the lack of control of their fabrication process with reflection high en…
We report on a systematic study of the growth of epitaxial TiO2 films deposited by pulsed laser deposition on Ti-terminated (001) SrTiO3 single crystals. By using in-situ reflection high energy electron diffraction, low energy electron diffraction, x-ray photoemission spectroscopy and scanning probe microscopy, we show that the stabilization of the anatase (001) phase is preceded by the growth of a pseudomorphic Sr-Ti-O intermediate layer, with a thickness between 2 and 4 nm. The data demonstrate that the formation of this phase is related to the activation of long range Sr migration from the …
We report the epitaxial growth of BiFeO3 by pulsed electron deposition and the resulting crystal quality, magnetic and nanoscale switching properties. X-ray diffraction shows high quality single phase, epitaxial (001) oriented films grown on SrTiO3 (001) substrates. Both field and temperature dependent magnetic properties reveal an antiferromagnetic behavior of the films. For the film with a SrRuO3 bottom electrode, an exchange-enhancement effect between antiferromagnetic BiFeO3 and ferromagnetic SrRuO3 was observed at low temperature. The piezoelectric force microscopy and switching spectrosc…
We present a combined study with conventional far-infrared and time-domain terahertz ellipsometry of the temperature dependent optical response of SrTiO3 thin films (85 and 8.5 nm) that are grown by pulsed-laser deposition on LSAT substrates. We demonstrate that terahertz ellipsometry is very sensitive to the optical response of these thin films, in particular, to the soft mode of SrTiO3. We show that for the 85 nm film the eigenfrequency of the soft mode is strongly reduced by annealing at 1200 C, whereas for the 8.5 nm film it is hardy affected. For the latter, after annealing the mode remai…
A series of 100 nm LaVO3 thin films have been synthesized on (001)-oriented SrTiO3 substrates using the pulsed laser deposition technique, and the effects of growth temperature are analyzed. Transport properties reveal a large electronic mobility and a non-linear Hall effect at low temperature. In addition, a cross-over from a semiconducting state at high-temperature to a metallic state at low-temperature is observed, with a clear enhancement of the metallic character as the growth temperature increases. Optical absorption measurements combined with the two-bands analysis of the Hall effect sh…
Epitaxial Mn-doped BiFeO3 (MBFO) thin films were grown on GaAs (001) substrate with SrTiO3 (STO) buffer layer by pulsed laser deposition. X-ray diffraction results demonstrate that the films show pure (00l) orientation, and MBFO(100)//STO(100), whereas STO (100)//GaAs (110). Piezoresponse force microscopy images and polarization versus electric field loops indicate that the MBFO films grown on GaAs have an effective ferroelectric switching. The MBFO films exhibit good ferroelectric behavior (2Pr ~ 92 μC/cm2 and 2EC ~ 372 kV/cm). Ferromagnetic property with saturated magnetization of 6.5 emu/cm…
The domain structures and dislocations in epitaxial thin films of La0.7Ca0.3MnO3 grown on SrTiO3 substrates by pulsed laser deposition were investigated using Bragg-contrast diffraction and high-resolution transmission electron microscopy. It revealed that the films contained the 1/2[100]o and 1/2[10-1]o types partial threading dislocations, the 90 degree - and 120 degree - types of twin- domain boundaries, and two types 1/2[010]o, 1/2[111]o, of antiphase boundaries, which are often observed in bulk materials. In addition, two types of superdislocations were detected; one consisted of two 1/2[…
Pulsed-laser deposition has been used to grow epitaxial thin films of the giant-dielectric-constant material CaCu_3Ti_4O_{12} on LaAlO_3 and SrTiO_3 substrates with or without various conducting buffer layers. The latter include YBa_2Cu_3O_7, La_{1.85}Sr_{0.15}CuO_{4+δ} and LaNiO_3. Above 100K - 150K the thin films have a temperature independent dielectric constant as do single crystals. The value of the dielectric constant is of the order of 1500 over a wide temperature region, potentially making it a good candidate for many applications. The frequency dependence of its dielectric properties …
Heterostructures and crystal interfaces play a major role in state-of-the-art semiconductor devices and play a central role in the field of oxide electronics. In oxides the link between the microscopic properties of the interfaces and bulk properties of the resulting heterostructures challenge our fundamental understanding. Insights on the early growth stage of interfaces and its influence on resulting physical properties are scarce -- typically the information is inferred from post growth characterization. Here, we report on real time measurements of the transport properties of SrTiO3-based h…
Our ability to design and fabricate electronic devices with reproducible properties using complex oxides is critically dependent on our ability to controllably synthesize these materials in thin-film form. Structure-property relationships are intimately tied to film and interface composition. Here we report on the effects of cation stoichiometry in LaCrO3 heteroepitaxial films prepared using molecular beam epitaxy. We show that LaCrO3 films grow pseudomorphically on SrTiO3(001) over a wide range of La-to-Cr atom ratios. However, the growth mode and structural quality are sensitive to the La-to…
Obtaining high-quality thin films of 5d transition metal oxides is essential to explore the exotic semimetallic and topological phases predicted to arise from the combination of strong electron correlations and spin-orbit coupling. Here, we show that the transport properties of SrIrO3 thin films, grown by pulsed laser deposition, can be optimized by considering the effect of laser-induced modification of the SrIrO3 target surface. We further demonstrate that bare SrIrO3 thin films are subject to degradation in air and are highly sensitive to lithographic processing. A crystalline SrTiO3 cap la…
The two-dimensional electron gas (2DEG) at oxides interfaces and surfaces has attracted large attention in physics and research due to its unique electronic properties and possible application in optoelectronics and nanoelectronics. The origin of 2DEGes at oxide interfaces has been attributed to the well known "polar catastrophe" mechanism. On the other hand, recently a 2DEG was also found on a clean SrTiO3(001) surface where it is formed due to oxygen vacancies. However, these 2DEG systems have been until now found mostly on atomically perfect crystalline samples usually grown by pulsed laser…
Complex oxide perovskites have been widely studied for their diverse functional properties. When dimensionally reduced to epitaxial thin films and heterostructures these properties are frequently tunable, and the symmetry-breaking inherent to thin film structures can result in the emergence of new, novel, phenomena and properties. However, the ability to control and harness these structures relies on an atomic-level understanding and control of the growth process, made challenging by the lack of suitable in situ compositional characterization tools. In this work, the compositional-dependence o…
Epitaxial (001)-, (118)-, and (104)-oriented Nd-doped Bi4Ti3O12 films have been grown by pulsed-laser deposition from a Bi4-xNdxTi3O12 (x=0.85) target on SrRuO3 coated single-crystal (100)-, (110)-, and (111)-oriented SrTiO3 substrates, respectively. X-ray diffraction illustrated a unique epitaxial relationship between film and substrate for all orientations. We observed a strong dependence of ferroelectric properties on the film orientation, with no ferroelectric activity in an (001)-oriented film; a remanent polarization, 2Pr, of 12 microC/cm2 and coercive field, Ec, of 120 kV/cm in a (118)-…
Thin film growth of ferroelectric or multiferroic materials on SrTiO3(111) with a buffer electrode has been hampered by the difficulty of growing flat electrodes on this polar orientation. We report on the growth and characterization of SrRuO3 thin films deposited by pulsed laser deposition on SrTiO3(111). We show that our SrRuO3(111) films are epitaxial and display magnetic bulk-like properties. Films presenting a thickness between 20 and 30nm are found to be very flat (with an RMS of about 0.5 nm) and therefore suitable as bottom electrodes in heterostructures.
Epitaxial thin films of REBa2Cu3O7-d (RE123, RE: rare earth) having a high entropy (HE) RE site were successfully fabricated on a SrTiO3 substrate by the pulsed laser deposition method. One to five RE elements are solved at the RE site, which results in an increase in configurational entropy of mixing (dSmix). Through the measurements of critical current density (Jc) by a magnetization and the Bean's model analysis, we found that the Jc of the HE films exceeds an order of 1.0 MA/cm2 under conditions of T < 20 K and H < 7 T. Since the HE effects have a potential to an improvement of irradiation…
We have investigated the magnetotransport properties of La0.7Sr0.3MnO3/BaTiO3 superlattices, grown on SrTiO3 substrate by pulsed laser deposition technique, both with current-in-plane and current-perpendicular-to-the-plane directions. Several features indicate the presence of magnetic inhomogeneities at the interfaces which is independent of BaTiO3 layer thickness variation. First, the magnetic property in the superlattices decreases. Second, a hysteresis in magnetoresistance due to the relaxation of the resistive state is observed. Third, a threshold under an applied magnetic field in the mag…
Heteroepitaxial growth of BaSnO$_3$ (BSO) and Ba$_{1-x}$La$_x$SnO$_3$ (x = 7 %) (LBSO) thin films on different perovskite single crystal (SrTiO$_3$ (001) and SmScO$_3$ (110)) substrates has been achieved by Pulsed Laser Deposition (PLD) under optimized deposition conditions. X-ray diffraction measurements indicate that the films on either of these substrates are relaxed due to the large mismatch and present a high degree of crystallinity with narrow rocking curves and smooth surface morphology while analytical quantification by proton induced x-ray emission (PIXE) confirms the stoichiometric L…
We grew SrTiO3 on SrTiO3 [001] by pulsed laser deposition, while observing x-ray diffraction at the (0 0 .5) position. The drop dI in the x-ray intensity following a laser pulse contains information about plume-surface interactions. Kinematic theory predicts dI/I = -4sigma(1-sigma), so that dI/I depends only on the amount of deposited material sigma. In contrast, we observed experimentally that |dI/I| < 4sigma(1-sigma), and that dI/I depends on the phase of x-ray growth oscillations. The combined results suggest a fast smoothing mechanism that depends on surface step-edge density.
We present a pulsed laser deposition (PLD) system that can monitor growth by simultaneously using in situ optical spectroscopic ellipsometry (SE) and reflection high-energy electron diffraction (RHEED). The RHEED precisely monitors the number of thin-film layers and surface structure during the deposition and the SE measures the optical spectra of the samples simultaneously. The thin-film thickness information obtained from RHEED facilitates the SE modeling process, which allows extracting the in situ optical spectra, i.e. the dielectric functions, of thin-films during growth. The in situ diel…