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Title: Substitution behavior of x(Na{sub 0.5}K{sub 0.5})NbO{sub 3}-(1 − x)BaTiO{sub 3} ceramics for multilayer ceramic capacitors by a near edge x-ray absorption fine structure analysis

Abstract

The doping effect of (Na{sub 0.5}K{sub 0.5})NbO{sub 3} (NKN) as alternatives for rare-earth elements on the electrical properties of BaTiO{sub 3} has been investigated, in terms of their substitution behavior. The dielectric constant of a specimen with x = 0.05 was about 79% higher than that of pure BaTiO{sub 3}, and the temperature coefficient of capacitance was satisfied by the X7R specification. The specimen with x = 0.05 showed the lowest tetragonality among the four compositions and had a fine grain size of <2 μm. Although the addition of NKN decreased the specimen's tetragonality, the electrical properties were enhanced by the formation of defect dipoles and conduction electrons, which resulted from an acceptor and donor substitution behavior. Through O K-edge near edge x-ray absorption fine structure spectroscopy, the practical substitution behavior was defined by the change in Ti 3d orbital states. The energy separation of the Ti 3d orbitals was more apparent with the specimen of x = 0.05, which is related to the donor level from the donor substitution of Nb{sup 5+} ion for Ti-sites. Therefore, the simultaneous substitution of Na{sup +}/K{sup +} and Nb{sup 5+} ions into BaTiO{sub 3} can improve dielectric properties, based on the charge-transfer process.

Authors:
; ;  [1]
  1. School of Materials Science and Engineering, Pusan National University, Busan 609-735 (Korea, Republic of)
Publication Date:
OSTI Identifier:
22303900
Resource Type:
Journal Article
Resource Relation:
Journal Name: Applied Physics Letters; Journal Volume: 104; Journal Issue: 26; Other Information: (c) 2014 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; ABSORPTION; ABSORPTION SPECTROSCOPY; BARIUM COMPOUNDS; CAPACITORS; CERAMICS; CRYSTAL DEFECTS; DIPOLES; FINE STRUCTURE; GRAIN SIZE; LAYERS; NIOBATES; PERMITTIVITY; POTASSIUM COMPOUNDS; RARE EARTHS; SODIUM COMPOUNDS; TEMPERATURE COEFFICIENT; TITANATES; X RADIATION; X-RAY SPECTROSCOPY

Citation Formats

Ha, Jooyeon, Ryu, Jiseung, and Lee, Heesoo, E-mail: heesoo@pusan.ac.kr. Substitution behavior of x(Na{sub 0.5}K{sub 0.5})NbO{sub 3}-(1 − x)BaTiO{sub 3} ceramics for multilayer ceramic capacitors by a near edge x-ray absorption fine structure analysis. United States: N. p., 2014. Web. doi:10.1063/1.4886579.
Ha, Jooyeon, Ryu, Jiseung, & Lee, Heesoo, E-mail: heesoo@pusan.ac.kr. Substitution behavior of x(Na{sub 0.5}K{sub 0.5})NbO{sub 3}-(1 − x)BaTiO{sub 3} ceramics for multilayer ceramic capacitors by a near edge x-ray absorption fine structure analysis. United States. doi:10.1063/1.4886579.
Ha, Jooyeon, Ryu, Jiseung, and Lee, Heesoo, E-mail: heesoo@pusan.ac.kr. Mon . "Substitution behavior of x(Na{sub 0.5}K{sub 0.5})NbO{sub 3}-(1 − x)BaTiO{sub 3} ceramics for multilayer ceramic capacitors by a near edge x-ray absorption fine structure analysis". United States. doi:10.1063/1.4886579.
@article{osti_22303900,
title = {Substitution behavior of x(Na{sub 0.5}K{sub 0.5})NbO{sub 3}-(1 − x)BaTiO{sub 3} ceramics for multilayer ceramic capacitors by a near edge x-ray absorption fine structure analysis},
author = {Ha, Jooyeon and Ryu, Jiseung and Lee, Heesoo, E-mail: heesoo@pusan.ac.kr},
abstractNote = {The doping effect of (Na{sub 0.5}K{sub 0.5})NbO{sub 3} (NKN) as alternatives for rare-earth elements on the electrical properties of BaTiO{sub 3} has been investigated, in terms of their substitution behavior. The dielectric constant of a specimen with x = 0.05 was about 79% higher than that of pure BaTiO{sub 3}, and the temperature coefficient of capacitance was satisfied by the X7R specification. The specimen with x = 0.05 showed the lowest tetragonality among the four compositions and had a fine grain size of <2 μm. Although the addition of NKN decreased the specimen's tetragonality, the electrical properties were enhanced by the formation of defect dipoles and conduction electrons, which resulted from an acceptor and donor substitution behavior. Through O K-edge near edge x-ray absorption fine structure spectroscopy, the practical substitution behavior was defined by the change in Ti 3d orbital states. The energy separation of the Ti 3d orbitals was more apparent with the specimen of x = 0.05, which is related to the donor level from the donor substitution of Nb{sup 5+} ion for Ti-sites. Therefore, the simultaneous substitution of Na{sup +}/K{sup +} and Nb{sup 5+} ions into BaTiO{sub 3} can improve dielectric properties, based on the charge-transfer process.},
doi = {10.1063/1.4886579},
journal = {Applied Physics Letters},
number = 26,
volume = 104,
place = {United States},
year = {Mon Jun 30 00:00:00 EDT 2014},
month = {Mon Jun 30 00:00:00 EDT 2014}
}
  • We report the piezoelectric and ferroelectric properties of (Na{sub 0.5}Bi{sub 0.5}TiO{sub 3}){sub x}-(BaTiO{sub 3}){sub y}-(Na{sub 0.5}K{sub 0.5}NbO{sub 3}){sub 1-x-y} ceramics for Na{sub 0.5}K{sub 0.5}NbO{sub 3} rich end of composition (x, y {<=} 0.04 mol. %). These compositions were found to exhibit significantly improved thermal stability of piezoresponse. Variation of dielectric constant as a function of temperature revealed that orthorhombic-tetragonal (T{sub o-t}) and tetragonal-cubic (T{sub c}) transition temperatures for these compositions were in the vicinity of 0 Degree-Sign C and 330 Degree-Sign C, respectively. Dynamic scaling and temperature dependent X-ray diffraction analysis were conducted. Results are discussed in terms of intrinsicmore » and extrinsic contributions to the piezoelectric response explaining the temperature dependent behavior.« less
  • Phase diagram of Bi{sub 0.5}Na{sub 0.5}TiO{sub 3}-BaTiO{sub 3}-K{sub 0.5}Na{sub 0.5}NbO{sub 3} ternary system has been analyzed and (0.94-x)BNT-0.06BT-xKNN (0.15{<=}x{<=}0.30) ceramics have been prepared and investigated. Pseudocubic structures were confirmed by x-ray diffractions and its preliminary Rietveld refinements. P-E, S-E, and S-P{sup 2} profiles (where P, E, and S denote polarization, electric field, and strain, respectively) indicate electrostrictive behavior of all ceramics. The compositions with x=0.20 and 0.25 show pure electrostrictive characteristics. The dissipation energy, electrostrictive strain, and electrostrictive coefficient have been determined and compared with other lead-free and lead-containing electrostrictors. The electrostrictive coefficient can reach as high as 0.026 m{supmore » 4}/C{sup 2}, about 1.5 times of the value of traditional Pb-based electrostrictors.« less
  • Highlights: • We fabricated lead-free (Na{sub 0.5}K{sub 0.5})NbO{sub 3} ceramics. • We studied the structural and electrical properties of 1 − x(Na{sub 0.5}K{sub 0.5})NbO{sub 3}–x(Sr{sub 0.5}Ca{sub 0.5})TiO{sub 3} ceramics. • The structural and electrical properties improved with increasing amount of (Sr{sub 0.5}Ca{sub 0.5})TiO{sub 3}. - Abstract: In this study, 1 − x(Na{sub 0.5}K{sub 0.5})NbO{sub 3}–x(Sr{sub 0.5}Ca{sub 0.5})TiO{sub 3} ceramics were fabricated using the conventional mixed oxide method. The effects of the addition of (Sr{sub 0.5}Ca{sub 0.5})TiO{sub 3} on the structural and electrical properties of the specimens were investigated for their application in piezoelectric devices. As the results of X-ray diffractionmore » analysis show, all specimens display the typical polycrystalline perovskite structure without the presence of the second phase. Sintered densities increased with an increase in the amount of (Sr{sub 0.5}Ca{sub 0.5})TiO{sub 3} added and the specimen with 0.08 mol% of (Sr{sub 0.5}Ca{sub 0.5})TiO{sub 3} added showed the maximum value of 4.54 g/cm{sup 3}. Both average grain size and densification increased with an increase in the amount of (Sr{sub 0.5}Ca{sub 0.5})TiO{sub 3}. The electromechanical coupling factor, dielectric constant ϵ{sub r}, dielectric loss tan δ, d{sub 33} and Curie temperature of the 0.92(Na{sub 0.5}K{sub 0.5})NbO{sub 3}–0.08(Sr{sub 0.5}Ca{sub 0.5})TiO{sub 3} specimens doped with 0.08 mol% of (Sr{sub 0.5}Ca{sub 0.5})TiO{sub 3} were 0.31, 1338, 0.021, 138 and 445 °C, respectively.« less
  • Lead-free piezoelectric ceramics (1-x-y)Bi{sub 0.5}Na{sub 0.5}TiO{sub 3}-xBaTiO{sub 3}-yK{sub 0.5}Na{sub 0.5}NbO{sub 3} (0.05{<=}x{<=}0.07 and 0.01{<=}y{<=}0.03), have been synthesized by a conventional solid state sintering method. The room temperature ferroelectric and piezoelectric properties of these ceramics were studied. Based on the measured properties, the ceramics were categorized into two groups: group I compositions having dominant ferroelectric order and group II compositions displaying mixed ferroelectric and antiferroelectric properties at room temperature. A composition from group II near the boundary between these two groups exhibited a strain as large as {approx}0.45% at an electric field of 8 kV/mm. Polarization in this composition was notmore » stable in that the piezoelectric coefficient d{sub 33} at zero electric field was only about 30 pm/V. The converse piezoelectric response becomes weaker when the composition deviated from the boundary between the groups toward either the ferroelectric or antiferroelectric compositions. These results were rationalized based on a field induced antiferroelectric-ferroelectric phase transition.« less
  • Structure and phase transitions of (1-y)((1-x)Bi 1/2Na 1/2TiO 3-xBi 1/2K 1/2TiO 3)-yK 0.5Na 0.5NbO 3 (x; y) piezoceramics (0.1 ≤ x ≤ 0.4; 0 ≤ y ≤ 0.05) were investigated by transmission electron microscopy, neutron diffraction, temperature-dependent x-ray diffraction, and Raman spectroscopy. The local crystallographic structure at room temperature (RT) does not change by adding K 0.5Na 0.5NbO 3 to Bi 1/2Na 1/2TiO 3-xBi 1/2K 1/2TiO 3 for x = 0.2 and 0.4. The average crystal structure and microstructure on the other hand develop from mainly long-range polar order with ferroelectric domains to short-range order with polar nanoregions displaying amore » more pronounced relaxor character. The (0.1; 0) and (0.1; 0.02) compositions exhibit monoclinic Cc space group symmetry, which transform into Cc + P4bm at 185 and 130 °C, respectively. This high temperature phase is stable at RT for the morphotropic phase boundary compositions of (0.1; 0.05) and all compositions with x = 0.2. For the compositions of (0.1; 0) and (0.1; 0.02), local structural changes on heating are evidenced by Raman; for all other compositions, changes in the long-range average crystal structure were observed.« less