Journal of the Korean Ceramic Society (한국세라믹학회지)

The Korean Ceramic Society (한국세라믹학회)
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Dielectric Properties and Ordering Structures of Pb(Fe1/2Ta1/2)O3-Pb(Fe1/2Nb1/2)O3 Solid Solutions

Pb(Fe1/2Ta1/2)O3-Pb(Fe1/2Nb1/2)O3 고용체의 유전특성 및 질서배열구조

  • Woo, Byong-Chul (Division of Chemical Metrology and Materials Evaluation, Korea Research Institute of Standards and Science) ;
  • Kim, Byung-Kook (Division of Materials, Korea Institute of Science and Technology) ;
  • Lee, Jong-Ho (Division of Materials, Korea Institute of Science and Technology) ;
  • Park, Hyun-Min (Division of Chemical Metrology and Materials Evaluation, Korea Research Institute of Standards and Science) ;
  • Kim, Byong-Ho (Division of Materials Science and Engineering, Korea University)
  • 우병철 (한국표준과학연구원 물질량표준부) ;
  • 김병국 (한국과학기술연구원 재료연구부) ;
  • 이종호 (한국과학기술연구원 재료연구부) ;
  • 박현민 (한국표준과학연구원 물질량표준부) ;
  • 김병호 (고려대학교 재료공학부)
  • Published : 2002.01.01
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Abstract

The Single phase $Pb(Fe_{1/2}Ta_{1/2})O_3$ (x=0.0∼1.0) solid solutions were successfully synthesized and their ordering structures as well as dielectric properties were investigated ${{r(Nb^{5+})=r(Ta^{5+})=0.78 {\AA},\;AW(Nb^{5+})=92.91,\;AW(Ta^{5+})=180.95}}$. While $Pb(Fe_{1/2}Ta_{1/2})O_3$ showed typical relaxor ferroelectric characteristics such as dielectric relaxation and diffuse phase transition, the sharpeness of the phase transition increased as $Ta^{5+}$ was replaced by $Nb^{5+}$ and finally $Pb(Fe_{1/2}Nb_{1/2})O_3$ showed normal ferroelectric characteristics with no dielectric relaxation. By using Raman spectroscopy, it was revealed that the $Fe^{3+}\;and\;Ta^{5+}\;of\;Pb(Fe_{1/2}Ta_{1/2})O_3$ were stoichiometrically 1:1 ordered within the short range which can be hardly probed even by TEM. Also, The degree of ordering in $Pb(Fe_{1/2}Ta_{1/2})O_3$ decreased as $Ta^{5+}$ was replaced by $Nb^{5+}$ and finally $Fe^{3+}\;and\;Nb^{5+}\;of\;Pb(Fe_{1/2}Nb_{1/2})O_3$ were completely disordered. The relaxor ferroelectric characteristics of $Pb(Fe_{1/2}Ta_{1/2})O_3$ could be correlated with the stoichiometric 1:1 ordering of B-site cations within the short range which can be hardly probed even by TEM. Also, the decrease of the relaxor ferroelectric characteristics with the replacement of $Ta^{5+}\;by\;Nb^{5+}$ could be correlated with the weakening of the ordering and the normal ferroelectric characteristics of $Pb(Fe_{1/2}Nb_{1/2})O_3$ could be correlated with the complete disordering of B-site cations.

$Pb(Fe_{1/2}Ta_{1/2})O_3$의 $Ta^{5+}$을 $Ta^{5+}$과 이온반경이 같고 원자량이 약 1/2배인 $Nb^{5+}$으로 치환한 $Pb{{Fe_{1/2}(Ta_(1-x)Nb_x)_{1/2}}O_3$ (x=0.0∼1.0) 고용체를 단일상으로 합성하여 그 유전특성 및 B자리 양이온 질서배열구조를 조사하였다. $Pb(Fe_{1/2}Ta_{1/2})O_3$는 유전완화현상 및 완만한 상전이가 뚜렷하게 관찰되는 전형적인 완화형 강유전특성을 보였지만, $Ta^{5+}$이 $Nb^{5+}$으로 치환됨에 따라 유전완화현상은 감소하고 상전이는 급격해져 결국 $Pb(Fe_{1/2}Nb_{1/2})O_3$는 유전완화현상이 전혀 관찰되지 않는 정상 강유전특성을 보였다. Raman 분광법에 의해 $Pb(Fe_{1/2}Ta_{1/2})O_3$의 $Fe^{3+}$과 $Ta^{5+}$은 XRD는 물론 TEM의 제한시야회절패턴으로도 검출하기 어려울 정도의 단거리영역에서 화학양론적으로 1:1 질서배열하고 있으며, $Ta^{5+}$이 $Nb^{5+}$으로 치환됨에 따라 $Fe^{3+}$과 ($Ta^{5+}-Nb^{5+}$) 간의 질서배열은 약화되어 결국 $Pb(Fe_{1/2}Nb_{1/2})O_3$의 $Fe^{3+}$과 $Nb^{5+}$은 완전 무질서배열하고 있음이 밝혀졌다. $Pb(Fe_{1/2}Ta_{1/2})O_3$의 완화형 강유전특성은 B자리 양이온들이 XRD는 물론 TEM의 제한시야회절패턴으로도 검출하기 어려울 정도의 단거리영역에서 화학양론적 1:1 질서배열을 하고 있는 것과, 또 $Pb(Fe_{1/2}Ta_{1/2})O_3$의 $Ta^{5+}$이 $Nb^{5+}$으로 치환됨에 따라 완화형 강유전특성이 감소되는 것은 이 질서배열이 약화되는 것과 그리고 $Pb(Fe_{1/2}Nb_{1/2})O_3$의 정상 강유전특성은 B자리 양이온들이 완전 무질서배열을 하고 있는 것과 연관지을 수 있었다.

Keywords

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