skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Growth of ferroelectric bismuth lanthanum nickel titanate thin films by rf magnetron sputtering

Abstract

The epitaxial growth, structural properties, and ferroelectric properties of bismuth lanthanum nickel titanate (Bi{sub 1-x}La{sub x}) (Ni{sub 0.5}Ti{sub 0.5})O{sub 3} (BLNT) thin films deposited on Pt(100)/MgO(100) substrates by rf magnetron sputtering have been investigated using x-ray diffraction, transmission electron microscope, and polarization-electric field hysteresis loop measurements. The ferroelectric BLNT(00l) phase with c-axis orientation and a single-phase tetragonal perovskite structure appeared at x{>=}0.3. The tetragonality (c/a) increased significantly from 1.004 to 1.028 with increasing La content. The fabricated BLNT films of x{>=}0.3 indicated the apparent fourfold rotational symmetry observed for a MgO(202) substrate, a bottom Pt(202) electrode, and a BLNT(101) ferroelectric film, based on {phi} scan measurements. These results imply that the present La-substituted BLNT films are grown heteroepitaxially at x{>=}0.3. It was confirmed that Bi in the BLNT films is in a trivalent state at A sites in the perovskite crystal, based on x-ray anomalous diffraction measurements and x-ray absorption near edge structure spectra. The sputtering technique using compacted powder targets designed by taking the bond dissociation energy of metal oxides into account provided epitaxial perovskite-structured BLNT thin films on Pt(100)/MgO(100) substrates. It is shown that the c-axis oriented epitaxial BLNT film exhibits a hysteresis loop shape with a P{submore » r} value of 12 {mu}C/cm{sup 2} that is comparable to typical high-performance Bi{sub 3.25}La{sub 0.75}Ti{sub 3}O{sub 12} (BLT) film.« less

Authors:
; ; ; ; ; ; ; ; ; ; ; ;  [1];  [2];  [2];  [2]
  1. Department of Materials Science and Chemistry, Graduate School of Engineering, University of Hyogo, 2167 Shosha, Himeji, Hyogo 671-2201 (Japan)
  2. (Japan)
Publication Date:
OSTI Identifier:
20982805
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Applied Physics; Journal Volume: 101; Journal Issue: 7; Other Information: DOI: 10.1063/1.2713352; (c) 2007 American Institute of Physics; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; ABSORPTION SPECTROSCOPY; BISMUTH COMPOUNDS; CHEMICAL BONDS; CRYSTAL GROWTH; DEPOSITION; DISSOCIATION ENERGY; EPITAXY; FERROELECTRIC MATERIALS; HYSTERESIS; LANTHANUM COMPOUNDS; MAGNESIUM OXIDES; NICKEL COMPOUNDS; PEROVSKITE; POLARIZATION; SPUTTERING; THIN FILMS; TITANATES; TRANSMISSION ELECTRON MICROSCOPY; X-RAY DIFFRACTION; X-RAY SPECTROSCOPY

Citation Formats

Kobune, Masafumi, Fukushima, Koji, Yamaji, Toru, Tada, Hideto, Yazawa, Tetsuo, Fujisawa, Hironori, Shimizu, Masaru, Nishihata, Yasuo, Matsumura, Daiju, Mizuki, Jun'ichiro, Yamaguchi, Hideshi, Kotaka, Yasutoshi, Honda, Koichiro, Department of Electrical Engineering and Computer Sciences, Graduate School of Engineering, University of Hyogo, 2167 Shosha, Himeji, Hyogo 671-2201, Synchrotron Radiation Research Center, Japan Atomic Energy Agency, Mikazuki, Sayo, Hyogo 679-5148, and Device and Materials Laboratories, Fujitsu Laboratories Ltd., 10-1 Morinosato-Wakamiya, Atsugi, Kanagawa 243-0197. Growth of ferroelectric bismuth lanthanum nickel titanate thin films by rf magnetron sputtering. United States: N. p., 2007. Web. doi:10.1063/1.2713352.
Kobune, Masafumi, Fukushima, Koji, Yamaji, Toru, Tada, Hideto, Yazawa, Tetsuo, Fujisawa, Hironori, Shimizu, Masaru, Nishihata, Yasuo, Matsumura, Daiju, Mizuki, Jun'ichiro, Yamaguchi, Hideshi, Kotaka, Yasutoshi, Honda, Koichiro, Department of Electrical Engineering and Computer Sciences, Graduate School of Engineering, University of Hyogo, 2167 Shosha, Himeji, Hyogo 671-2201, Synchrotron Radiation Research Center, Japan Atomic Energy Agency, Mikazuki, Sayo, Hyogo 679-5148, & Device and Materials Laboratories, Fujitsu Laboratories Ltd., 10-1 Morinosato-Wakamiya, Atsugi, Kanagawa 243-0197. Growth of ferroelectric bismuth lanthanum nickel titanate thin films by rf magnetron sputtering. United States. doi:10.1063/1.2713352.
Kobune, Masafumi, Fukushima, Koji, Yamaji, Toru, Tada, Hideto, Yazawa, Tetsuo, Fujisawa, Hironori, Shimizu, Masaru, Nishihata, Yasuo, Matsumura, Daiju, Mizuki, Jun'ichiro, Yamaguchi, Hideshi, Kotaka, Yasutoshi, Honda, Koichiro, Department of Electrical Engineering and Computer Sciences, Graduate School of Engineering, University of Hyogo, 2167 Shosha, Himeji, Hyogo 671-2201, Synchrotron Radiation Research Center, Japan Atomic Energy Agency, Mikazuki, Sayo, Hyogo 679-5148, and Device and Materials Laboratories, Fujitsu Laboratories Ltd., 10-1 Morinosato-Wakamiya, Atsugi, Kanagawa 243-0197. Sun . "Growth of ferroelectric bismuth lanthanum nickel titanate thin films by rf magnetron sputtering". United States. doi:10.1063/1.2713352.
@article{osti_20982805,
title = {Growth of ferroelectric bismuth lanthanum nickel titanate thin films by rf magnetron sputtering},
author = {Kobune, Masafumi and Fukushima, Koji and Yamaji, Toru and Tada, Hideto and Yazawa, Tetsuo and Fujisawa, Hironori and Shimizu, Masaru and Nishihata, Yasuo and Matsumura, Daiju and Mizuki, Jun'ichiro and Yamaguchi, Hideshi and Kotaka, Yasutoshi and Honda, Koichiro and Department of Electrical Engineering and Computer Sciences, Graduate School of Engineering, University of Hyogo, 2167 Shosha, Himeji, Hyogo 671-2201 and Synchrotron Radiation Research Center, Japan Atomic Energy Agency, Mikazuki, Sayo, Hyogo 679-5148 and Device and Materials Laboratories, Fujitsu Laboratories Ltd., 10-1 Morinosato-Wakamiya, Atsugi, Kanagawa 243-0197},
abstractNote = {The epitaxial growth, structural properties, and ferroelectric properties of bismuth lanthanum nickel titanate (Bi{sub 1-x}La{sub x}) (Ni{sub 0.5}Ti{sub 0.5})O{sub 3} (BLNT) thin films deposited on Pt(100)/MgO(100) substrates by rf magnetron sputtering have been investigated using x-ray diffraction, transmission electron microscope, and polarization-electric field hysteresis loop measurements. The ferroelectric BLNT(00l) phase with c-axis orientation and a single-phase tetragonal perovskite structure appeared at x{>=}0.3. The tetragonality (c/a) increased significantly from 1.004 to 1.028 with increasing La content. The fabricated BLNT films of x{>=}0.3 indicated the apparent fourfold rotational symmetry observed for a MgO(202) substrate, a bottom Pt(202) electrode, and a BLNT(101) ferroelectric film, based on {phi} scan measurements. These results imply that the present La-substituted BLNT films are grown heteroepitaxially at x{>=}0.3. It was confirmed that Bi in the BLNT films is in a trivalent state at A sites in the perovskite crystal, based on x-ray anomalous diffraction measurements and x-ray absorption near edge structure spectra. The sputtering technique using compacted powder targets designed by taking the bond dissociation energy of metal oxides into account provided epitaxial perovskite-structured BLNT thin films on Pt(100)/MgO(100) substrates. It is shown that the c-axis oriented epitaxial BLNT film exhibits a hysteresis loop shape with a P{sub r} value of 12 {mu}C/cm{sup 2} that is comparable to typical high-performance Bi{sub 3.25}La{sub 0.75}Ti{sub 3}O{sub 12} (BLT) film.},
doi = {10.1063/1.2713352},
journal = {Journal of Applied Physics},
number = 7,
volume = 101,
place = {United States},
year = {Sun Apr 01 00:00:00 EDT 2007},
month = {Sun Apr 01 00:00:00 EDT 2007}
}
  • Thermally stimulated currents (TSCs) are measured in amorphous barium titanate thin films deposited by the rf sputtering technique. The TSC global curve is composed of three overlapping peaks in the 0-200 deg. C temperature range. At 50 deg. C, a first TSC peak is observed that can be related to a shallow-trap level. A second peak due to a dipolar polarization process is observed at 95 deg. C. Finally, a third peak appears at 140 deg. C that is ascribed to the oxygen vacancy motion and their accumulation at electrodes. The different peaks constituting the global TSC spectrum are separatelymore » studied by the fractional polarization technique in order to analyze their fine structures and to determine their activation energies.« less
  • Bi{sub 3.25}La{sub 0.75}Ti{sub 3}O{sub 12} (BLT) thin films with Bi{sub 2}O{sub 3} seed layers were prepared on Pt(111)/Ti/SiO{sub 2}/Si substrate by rf-magnetron sputtering method. The effect of annealing procedure, thickness, and position of Bi{sub 2}O{sub 3} seed layer on the structural and electrical properties of BLT thin film was investigated. When using a two-step annealing procedure, the x-ray diffraction pattern indicated that BLT thin film with a Bi{sub 2}O{sub 3} seed layer showed c-axis preference orientation. Compared with Pt/BLT/Bi{sub 2}O{sub 3}/Pt structure film, the Pt/Bi{sub 2}O{sub 3}/BLT/Bi{sub 2}O{sub 3}/Pt structure film showed higher oriented to c direction. The ferroelectric propertymore » of BLT thin film improved remarkably with the incorporation of Bi{sub 2}O{sub 3} seed layer. Under the applied voltage of 14 V, the remnant polarization and coercive voltage of the Bi{sub 2}O{sub 3}/BLT/Bi{sub 2}O{sub 3} capacitor with 18-nm-thick Bi{sub 2}O{sub 3} seed layer were 45.2 {mu}C/cm{sup 2} and 9.2 V, respectively. Moreover, the Pt/Bi{sub 2}O{sub 3}/BLT/Bi{sub 2}O{sub 3}/Pt film with 18-nm-thick Bi{sub 2}O{sub 3} seed layers exhibited good fatigue endurance even after 6x10{sup 9} switching cycles, which was attributed to the double-sided Bi{sub 2}O{sub 3} layer. They decreased the grain boundary density by enhancing the grain size of BLT film and enhanced the c-axis preferential orientation. Compared with BLT film deposited directly on Pt, double-sided Bi{sub 2}O{sub 3} layer would greatly enhance the leakage current resistance of the BLT film.« less
  • Highlights: • High-quality PMN-PT 90/10 RFE thin films were prepared by RF magnetron sputtering. • The maximum discharged density of 31.3 J/cm{sup 3} was obtained in the 750-nm-thick film. • PMN-PT RFE films might be a promising material for energy-storage application. - Abstract: 0.9Pb(Mg{sub 1/3}Nb{sub 2/3})O{sub 3}-0.1PbTiO{sub 3} (PMN-PT 90/10) relaxor ferroelectric thin films with different thicknesses were deposited on the LaNiO{sub 3}/Si (100) by the radio-frequency (RF) magnetron sputtering technique. The effects of thickness and deposition temperature on the microstructure, dielectric properties and the energy-storage performance of the thin films were investigated in detail. X-ray diffraction spectra indicated thatmore » the thin films had crystallized into a pure perovskite phase with a (100)-preferred orientation after annealed at 700 °C. Moreover, all the PMN-PT 90/10 thin films showed the uniform and crack-free surface microstructure. As a result, a larger recoverable energy density of 31.3 J/cm{sup 3} was achieved in the 750-nm-thick film under 2640 kV/cm at room temperature. Thus, PMN-PT 90/10 relaxor thin films are the promising candidate for energy-storage capacitor application.« less
  • PLZT(X/0/100) thin films on MgO(100), Pt/Ti/MgO(100), and Pt/Ti/Si(100) have been prepared by RF-magnetron sputtering process from sintered target with compositions of PLZT(X/0/100), where X = 5, 10, and 15, respectively. The effects of substrate temperature, substrate and gas pressure on deposited thin films were studied. Crystalline and surface characterization was analyzed using XRD, SEM, AES, and AFM. X-ray rocking curves were measured to examine the film orientation. It was observed that the gas pressure was the dominant influence on having (001) preferred orientation. As a result, the degree of c-axis orientation increased as gas pressure decreased.
  • Epitaxial lead zirconium titanate (PZT) (001) thin films with a Pt bottom electrode were deposited by rf sputtering onto Si(001) single crystal substrates with a Ag buffer layer. Both PZT(20/80) and PZT(53/47) samples were shown to consist of a single perovskite phase and to have the (001) orientation. The orientation relationship was determined to be PZT(001)[110](parallel sign)Pt(001)[110](parallel sign)Ag(001)[110](parallel sign)Si(001)[110]. The microstructure of the multilayer was studied using transmission electron microscopy (TEM). The electron diffraction pattern confirmed the epitaxial relationship between each layer. The measured remanent polarization P{sub r} and coercive field E{sub c} of the PZT(20/80) thin film were 26more » {mu}C/cm{sup 2} and 110 kV/cm, respectively. For PZT(53/47), P{sub r} was 10 {mu}C/cm{sup 2} and E{sub c} was 80 kV/cm.« less