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Artificial construction of SrO/(La, Sr)MnO3 layered perovskite superlattice by laser molecular-beam epitaxy

Appl. Phys. Lett. 76, 3618 (2000); doi:10.1063/1.126725


Epitaxial thin films of layered perovskite (La, Sr)3Mn2O7 have been artificially grown by atomic-layer stacking of SrO and (La, Sr)MnO 3 [artificial SrO/(La, Sr)MnO3 superlattice] using laser molecular-beam epitaxy on an SrTiO 3(001) substrate at low processing temperature. Reflection high-energy electron diffraction patterns indicate the flat surface of the films and the layer-by-layer growth mode. X-ray diffraction patterns confirm that c-axis-oriented Ruddlesden Popper layered (La, Sr)3Mn2O7 thin films can be grown at a substrate temperature as low as 580 C. The resulting film exhibited ferromagnetism with a Curie temperature of 75 K. 2000 American Institute of Physics.

Polarization rotation in epitaxially strained perovskite-oxide superlattices


Nakhmanson, Serge American Physical Society, 2009 APS March Meeting, March 16-20, 2009, abstract #B10.008 Utilizing first-principles computational techniques, we have mapped out -point structural instabilities in (BaTiO3)8/(SrTiO3)4 superlattices held at varying degrees of epitaxial strain and constrained to P4mm symmetry with fully developed polarization in the out-of-plane direction. We find that at compressive strains larger than -0.5% (with respect to a fully relaxed P4mm structure) the superlattices exhibit no structural instabilities. However, at a smaller compressive strain, an in-plane ferroelectric instability emerges in the SrTiO3 layers. This instability is then complemented by a similar instability in the BaTiO3 layers that develops at tensile strain of more than 0.2%, suggesting nonzero polarization components for both in- and out-of-plane directions throughout the whole superlattice.

Perovskite superlattices as tunable microwave devices


NASA Tech Briefs, May 2003

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Interfacial interactions between paraelectric materials induce quasi-ferroelectric behavior. John H. Glenn Research Center, Cleveland, Ohio. Experiments have shown that superlattices that comprise alternating epitaxial layers of dissimilar paraelectric perovskites can exhibit large changes in permittivity with the application of electric fields. The superlattices are potentially useful as electrically tunable dielectric components of such microwave devices as filters and phase shifters. The electrically tunable materials heretofore used in some microwave devices exhibit strong temperature dependences of dielectric properties and high microwave losses. Previous efforts to overcome these undesired effects have involved the addition of various dopants to SrTiO^sub 3^, BaTiO^sub 3^, and Sr^sub x^Ba^sub x-1^TiO^sub 3^. Despite the amount of research in this area, results have been disappointing. The present superlattice approach differs fundamentally from the prior use of homogeneous, isotropic mixtures of base materials and dopants. A superlattice can comprise layers of two or more perovskites in any suitable sequence (e.g., ABAB..., ABCDABCD..., ABACABACA...). Even though a single layer of one of the perovskites by itself is not tunable, the compositions and sequence of the layers can be chosen so that (1) the superlattice exhibits low microwave loss and (2) the interfacial interaction between at least two of the perovskites in the superlattice renders either the entire superlattice or else at least one of the perovskites tunable. The perovskites investigated experimentally for use in superlattices include SrTiO^sub 3^, SrCeO^sub 3^, SrZrO^sub 3^, BaTiO^sub 3^, BaZrO^sub 3^, CaZrO^sub 3^, and LaAlO^sub 3^. Superlattices for the experiments were fabricated by pulsed laser deposition onto mostly LaAlO^sub 3^ substrates; a few specimens were prepared on SrTiO^sub 3^ substrates. Microwave filters containing superlattices were also fabricated. The superlattices were evaluated with respect to structure, composition, and dielectric properties. Analysis of the observations made in the experiments led to the following conclusions: * Large tuning was observed in capacitors made from some superlattices (see figure). Ferroelectricity induced by lattice-mismatch strain in superlattices has been tentatively identified as the cause of tunability in the otherwise nontunable paraelectric perovskite constituents. * Some of the superlattices exhibited positive d[epsilon]/dE, where [epsilon] is permittivity and E is the magnitude of an applied electric field. This stands in contrast to the negative values of d[epsilon]/dE typically observed in perovskites. * Superlattices can be made to exhibit weak temperature dependences of tunability. For example, one SrTiO^sub 3^/ BaZrO^sub 3^ superlattice was found to exhibit a tunability of 38 percent at both room temperature and at 77 K. In contrast, a typical ferroelectric material is tunable in only a narrow temperature range near a phase transition. Superlattices with weak temperature dependence of tunability could be attractive materials for situations in which precise control of temperature would be either impossible or too expensive.

* In tests on coplanar-waveguide microwave filters containing perovskite superlattices of a given total thickness, dielectric losses were found to be smaller than those in filters containing single SrTiO^sub 3^ films of the same total thickness. This work was done by H. M. Christen and K. S. Harshavardhan of Neocera, Inc., for Glenn Research Center. For further information, access the Technical Support Package (TSP) free on-line at www.nasatech. com/tsp under the Materials category. Inquiries concerning rights for the commercial use of this invention should be addressed to NASA Glenn Research Center, Commercial Technology Office, Attn: Steve Fedor, Mail Stop 4-8, 21000 Brookpark Road, Cleveland, Ohio 44135. Refer to LEW-16938.
Copyright Associated Business Publications May 2003 Provided by ProQuest Information and Learning Company. All rights Reserved

Dielectric and Optical Properties of Perovskite-Type Artificial Superlattices

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Author(s): Takakiyo Harigai, Song-Min Nam, Hirofumi Kakemoto, Satoshi Wada, Keisuke Saito, Takaaki Tsurumi Tokyo Institute of Technology BaTiO3/SrTiO3, BaTiO3/BaZrO3, and SrZrO3/SrTiO3 artificial superlattices were fabricated on SrTiO3 substrates by the molecular beam epitaxy (MBE) process. The stacking periodicity of each layer was varied from 1 unit cell to 40 unit cells, and the total thickness was fixed at 80 unit cells. In-situ reflection high-energy electron diffraction (RHEED) and xray diffraction (XRD) clearly shows the formation of the superlattice structure. Their lattice parameters obtained from the reciprocal space mapping measurement indicated that the lattice distortion was dependent on the stacking periodicity. The capacitance and the complex admittance of the superlattices were measured with interdigital electrodes by an impedance analyzer up to 110 MHz. It was found that the dielectric permittivity changed with the superlattice periodicity. The Q-V measurement results showed clear hysteresis curves and this suggested that ferroelectricity was induced into the SrZrO3/SrTiO3 superlattices despite a combination between paraelectrics/paraelectrics.

Advanced Functional Materials


Volume 18 Issue 24, Pages 3892 - 3906

Published Online: 10 Nov 2008 Copyright 2009 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
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Feature Article
Functional Perovskites - From Epitaxial Films to Nanostructured Arrays Ionela Vrejoiu, Marin Alexe, Dietrich Hesse *, Ulrich Gsele Max Planck Institute of Microstructure Physics Weinberg 2, 06120 Halle (Germany) email: Dietrich Hesse (hesse@mpi-halle.de)

Correspondence to Dietrich Hesse, Max Planck Institute of Microstructure Physics Weinberg 2, 06120 Halle (Germany).
*

The authors are thankful to Drs. Dinghua Bao, Balaji I. Birajdar, Ksenia Boldyreva, Ming-Wen Chu, Hee Han, Catalin Harnagea, Chun-Lin Jia (FZ Jlich, Germany), Sergei Kalinin (Oak Ridge Natl. Lab., USA), Clemens von Korff Schmising (Max Born Institute Berlin, Germany), Ho Nyung Lee, Sung Kyun Lee, Woo Lee, Gwenael Le Rhun, Lifeng Liu, Andriy Lotnyk, Wenhui Ma, I. Burc Misirlioglu, Kornelius Nielsch, Lucian Pintilie, Eckhard Pippel, Brian Rodriguez, Stephan Senz, Annette Setzer (Leipzig University, Germany), Steffen Schmidt, Roland Scholz, Izabella Szafraniak, Nikolai D. Zakharov, Michael Ziese (Leipzig University, Germany), and Yinilian Zhu for their respective most valuable experimental contributions, as well as for many fruitful discussions. Sincere thanks are due to Professors James F. Scott (Cambridge University, UK), Ramamoorthy Ramesh (University of Berkeley, USA), Sunggi Baik (POSTECH, Korea), Matias Bargheer (Potsdam University, Germany) and Knut Urban (FZ

Jlich, Germany) for many stimulating discussions and fruitful cooperations. This work has been funded by the Max Planck Society, the German Science Foundation (DFG, FOR 404 and SFB 762), Volkswagen Foundation (Ferroelectric hybrides), the German Federal Ministry of Research (BMBF, 13N7986), the Alexander von Humboldt Foundation, and various European Union programs.

Funded by: Max Planck Society German Science Foundation (DFG); Grant Number: FOR 404, SFB 762 Volkswagen Foundation (Ferroelectric hybrides) German Federal Ministry of Research (BMBF); Grant Number: 13N7986 Alexander von Humboldt Foundation
Keywords ferroelectrics nanostructures perovskites piezoelectrics thin films Abstract Functional perovskite materials gain increasing significance due to their wide spectrum of attractive properties, including ferroelectric, ferromagnetic, conducting and multiferroic properties. Due to the developments of recent years, materials of this type can conveniently be grown, mainly by pulsed laser deposition, in the form of epitaxial films, multilayers, superlattices, and wellordered arrays of nanoislands. These structures allow for investigations of preparation-microstructure-property relations. A wide variation of the properties is possible, determined by strain, composition, defect contents, dimensional effects, and crystallographic orientation. An overview of our corresponding work of recent years is given, particularly focusing on epitaxial films, superlattices and nanoisland arrays of (anti)ferroelectric and multiferroic functional perovskites.

Structural and dielectric properties of perovskite-type artificial superlattices

Auteur(s) / Author(s)
HARIGAI Takakiyo (1) ; NAM Song-Min (1) ; KAKEMOTO Hirofumi (1) ; WADA Satoshi (1) ; SAITO Keisuke (2) ; TSURUMI Takaaki (1) ;

Affiliation(s) du ou des auteurs / Author(s) Affiliation(s)


(1)

Department of Metallurgy and Ceramics Science, Graduate School of Science and Engineering, Tokyo Institute of Technology, 2-12-1 Ookayama, Meguro-ku, Tokyo 1528552, JAPON (2) BRUKER AXS K. K., 3-9-A Moriya-cho, Kanagawa-ku, Yokohama-shi, Kanagawa 2210022, JAPON

Rsum / Abstract

BaTiO3/SrTiO3, SrZrO3/SrTiO3 and BaTiO3/BaZrO3 artificial superlattices were fabricated by the molecular beam epitaxy process. X-ray diffraction (XRD) reciprocal space mapping measurement was performed using high-resolution XRD. In all artificial superlattices, the superlattices with the 10-periodic structure showed the clear satellite peaks in the XRD pattern and were mostly distorted in the direction of film thickness. Superlattices with the 10periodic structure showed a high dielectric permittivity of r=33,000 or artificially induced ferroelectricity. It was clarified that the anisotropic lattice distortion introduced by the strains due to the lattice mismatch was the origin of the unique dielectric characteristics of artificial superlattices.

Revue / Journal Title


Thin solid films ISSN 0040-6090 CODEN THSFAP

Source / Source
Congrs International Symposium on the Manipulation of Advanced Smart Materials, Nara , JAPON (26/05/2005) 2006, vol. 509, no 1-2 (236 p.) [Document : 5 p.] (15 ref.), pp. 13-17 [5 page(s) (article)]

Langue / Language
Anglais

Editeur / Publisher
Elsevier Science, Lausanne, SUISSE (1967) (Revue)

Epitaxial Oxides and Heterostructures


The effect of strain on properties of perovskites (Collaboration with H.N. Lee, D.H. Kim, and C.M Rouleau) Epitaxial thin films are strongly affected by lattice strain. For KNbO3 layers in superlattices with paraelectric KTaO3, an increase of the ferroelectric transition temperature by 100 degrees is observed (Appl. Phys. Lett., 1998). More strikingly, room-temperature ferroelectricity is observed in nominally paraelectric SrTiO3 layers when subjected to in-plane tensile strain (Phys. Rev. B, 2003). A surprisingly weak response is observed in other types of ferroelectrics: in PbZr0.2Ti0.8O3 (Phys. Rev. Lett., 2007) and BiFeO3 (Appl. Phys. Lett., 2008), the polarization remains almost unchanged when the amount of strain is modified by varying the film thickness. In charge-ordered manganites, subtle effects of strain magnitude and symmetry are observed by comparing results on differentsubstrates and substrate orientations (Appl. Phys. Lett., 2006). Atomic-scale control in perovskite superlattices (Film growth with H.N. Lee and C.M. Rouleau; microscopy: M.F. Chisholm and M. Varela) The effects of interfaces and spatial confinement play the most crucial role in determining the properties of nanostructured complex materials. Their study requires unprecedented control over interfacial quality. We are applying PLD to the growth of atomic-scale perovskite superlattices with atomically flat interfaces, obtained at sufficiently high oxygen pressures to yield bulk-like properties, without requiring post-annealing. The resulting crystalline quality was previously achieved only in lowpressure molecular-beam epitaxy approaches (see below). PLD can also yield very specific samples, such as the CaTiO3 structures used to demonstrate single-atom sensitivity of LaEELS spectroscopic imaging in a scanning transmission electron microscope (Phys. Rev. Lett., 2004). Non-inversion symmetric artificial crystals (Film growth: H.N. Lee with C.M. Rouleau; microscopy: M.F. Chisholm)

The breaking of inversion symmetry plays a key role in functional materials, yielding properties like ferroelectricity and magnetism. However, the permanent removal of inversion symmetry due to an asymmetric arrangement of elements within a material is rarely observed in conventional materials. Three-component superlattices (TCSs) (stackings of the type A-B-C-A-B-C) allow us to study the effects of asymmetry on ferroelectric properties in perovskite materials (Nature, 2005).

Stability of SrRuO3 films (Film growth and AFM investigation: H.N. Lee) SrRuO3 is widely used as bottom electrode for the measurement of physical properties in complex oxides. Our work has shown that the surface of SrRuO3 films is stable only in a limited range of the temperature oxygen pressure phase space (Appl. Phys. Lett., 2004). Ferroelectricity in perovskites superlattices Size effects and long-range interactions can be studied carefully in epitaxial heterostructures containing paraelectric and/or ferroelectric perovskites. In the case of KTaO3/KNbO3 superlattices, we have shown that the ferroelectric transition temperature converges towards that of the corresponding alloy as the layers become thinner (Appl. Phys. Lett., 1998), while the local crystalline structure (as probed by EXAFS) in the lowtemperature phase remains distinctly different (J. Electroceram., 2000). In heterostructures of SrTiO3 and BaZrO3 two non-ferroelectric materials characteristics of room-temperature ferroelectricity and of anti-ferroelectricity are observed depending on the superlattice periodicity (Phys. Rev. B, 2003). Quantum criticality in (CaxSr1-x)RuO3 (Film growth with I. Ohkubo, now at Tokyo University; characterization with P. Khalifah, now at University of Massachusetts) Systems exhibiting Non-Fermi Liquid (NFL) behavior, i.e. metals in which the low-temperature electronic behavior differs from that of the Fermi Liquid model, are rare exceptions to the vast majority of known materials. One potential route for finding NFL behavior is tuning a system to the vicinity of a quantum phase transition (QPT), a regime where the length scale of electronic fluctuations are diverging as the precise end point of the quantum phase transition is approached. Using PLD, thin film alloys of CaRuO3 and ferromagnetic SrRuO3 can be compositionally tuned to exhibit such a QPT (Phys. Rev. B, 2004).