リラクサの高誘電率発生の機構解明

• Project/Area Number: 12134202
• Research Category: Grant-in-Aid for Scientific Research on Priority Areas
• Allocation Type: Single-year Grants
• Review Section: Science and Engineering
• Research Institution: Gifu University
• Principal Investigator: 安田 直彦 岐阜大学, 工学部, 教授 (90021625)
• Co-Investigator(Kenkyū-buntansha): 大和 英弘 岐阜大学, 工学部, 助手 (70270973) ; 岩田 真 名古屋工業大学, 工学部, 助教授 (40262886) ; 前田 雅輝 名古屋工業大学, 工学部, 助教授 (10091745)
• Project Period (FY): 2000 – 2003
• Project Status: Completed (Fiscal Year 2003)
• Budget Amount: ¥38,400,000 (Direct Cost: ¥38,400,000); Fiscal Year 2003: ¥14,400,000 (Direct Cost: ¥14,400,000); Fiscal Year 2002: ¥12,100,000 (Direct Cost: ¥12,100,000); Fiscal Year 2001: ¥11,900,000 (Direct Cost: ¥11,900,000)
• Keywords: リラクサー強誘電体 / 固溶体 / 単結晶 / 高誘電率 / ドメインウオール構造 / 光バルブ誘電率制御素子 / キュリー温度 / AFM像 / リラクサ強誘電体 / モルフォトロッピク相境界 / モザイク結晶 / 不均一構造 / AFM観察 / 微小強誘電体ドメイン / インプリント効果 / 静水圧力効果 / 疲労効果の少ないFERAM / モルフォトロピック相境界 / ラマン散乱 / 電子線回折 / 電気光学応答 / エンジニアードドメイン構造 / 誘電率 / エンジニアードドメイン / 抗電界 / 微小極性領域 / 化学的秩序領域 / 電子顕微鏡像 / ラマン散乱解析

Research Abstract

リラクサ強誘電体固溶体(1-x)Pb(Mg_<1/3>Nb_<2/3>)O_3(PMN)-xPbTiO_3(PT)のあるPT組成範囲(0.1<x<0.2)に於いてrhombohedral(001)板に直流電界が印加されると、誘電率及びドメイン構造の電界依存性から、最初電界増加に伴い高誘電率領域から低誘電率領域へと電界誘起転移が生じ、同時に暗視野(光遮断)状態から明視野(光通過)状態へとドメイン構造も変化する。最初の暗視野状態は偏光顕微鏡のステイジの回転に対しても暗視野のままである。一旦電界により、低誘電率領域で光通過領域のメモリ状態へ移ると、誘電率、ドメイン構造はメモリされたままになる。ドメイン構造には<001>あるいは<010>方向に沿ったドメインウオールが見られ、電界極性反転による分極反転に伴い坑電界に対応して<001>あるいは<010>方向に沿ったドメインウオールが出現し、この時小さな誘電率異常が見られる。一旦分極が揃うとエンジニアードドメイン配置であるので安定なドメイン構造になり誘電率変化も少ない。この試料をキュリー温度まで上げて室温まで戻した状態の誘電率は高誘電率領域に戻り、偏光顕微鏡下での暗視野像はステイジの回転に対して暗視野像のままでas-grownの状態に戻っている。偏光顕微鏡のハロゲンランプは540nmのグリーンの波長を中心に400nmから600nmの範囲の光に対して暗視野になっておりリラクサーのドメインサイズはこれ以下であると考えられ、電顕によるドメインサイズ200nm以下の報告もある。このことからリラクサー強誘電体固溶体には光バルブ誘電率制御素子として使用可能であることが分かる。この事実を特許として出願した。更に、リラクサ強誘電体混晶Pb(Zn_<1/3>Nb_<2/3>)O_3-PbTiO_3のうち、正方晶相を示すPZN-20%PTと、室温で菱面体晶相を示し濃度相境界に近いPZN-8%PTのエッチング処理表面のAFM観察を行った。PZN-20%PTでは、90°および180°ドメインウォール構造が観察できた。PZN-8%PTでは、(001),(110),(111)に垂直な表面の観察から、180°,109°,71°のドメインウォール構造が観察できた。これらのドメインウォール構造の解析では、弾性的な条件であるSaprielの理論と、ドメインウォール表面で分極電荷が存在しないという電気的な条件の両方を満たしていることが確認できた。PZN-8%PTにおいてチャージドウォールは存在しない。PZN-8%PTの濃度相境界における正方晶相と菱面体晶相の相転移は、散漫な相転移であることが指摘されているが、局所的にはシャープな相転移をし、転移温度が場所に依存して分布していることがわかった。また、室温でのドメイン-ウォール構造は、通常の強誘電体と同様に古典論によって理解できることを実験的に示した。

Research Products

• [Publications] N.Yasuda, N.Uemura, Y.Ozaki, H.Ohwa, M.Iwata, Y.Ishibashi: "Domain observation in Pb(In_<1/2>Nb_<1/2>)O_3-PbTiO_3 solid solutions near morphotropic phase boundary by polarizing microscope."Transactions of Material Research Society of Jpn.. 28(1). 161-164 (2003)
• [Publications] M.Iwata, K.Katsuraya, M.Maeda, I.Suzuki, N.Yasuda, Y.Naruse, H.Orihara, Y.Ishibashi: "Domain-wall observation in Pb(Zn_<1/3>Nb_<2/3>)O_3-PbTiO_3 solid solutions by AFM."Transactions of Material Research Society of Jpn.. 28. 145-147 (2003)
• [Publications] H.Ohwa, N.Yasuda, M.Iwata, H.Orihara, Y.shibashi: "Pressure effect of dielectric property in solid solutions (1-x)Pb(Mg_<1/3>Nb_<2/3>)O_3-xPbZrO_3."Journal of Korean Physical Socciety. 42. S1270-S1274 (2003)
• [Publications] N.Yasuda, N.Uemura, H.Ohwa, Y.Yamashita, M.Iwata, M.Maeda, I.Suzuki, Y.Ishibashi: "Domain observation in PIN-PT mixed crystal near morphotropic phase boundary."Journal of Korean Physical Socciety. 42. S1261-S1265 (2003)
• [Publications] N.Yasuda, A.Nakada, R.Ozao, H.Ohwa, K.Fujita, M.Iwata, M.Maeda, I.Suzuki, Y.Ishibashi: "The relation between polarization and electric field for the phase transition from antiferroelectric to ferroelectric one of solid solutions (1-x)Pb(Sc_<1/2>Ta_<1/2>)O_3-xPbZrO_3(0.8<x<1)."Journal of Korean Physical Socciety. 42. S1046-S1050 (2003)
• [Publications] M.Iwata, M.Maeda, I.Suzuki, H.Ohwa, N.Yasuda, Y.Ishibashi: "Observation of domain-wall structure in Pb(Zn_<1/3>Nb_<2/3>)O_3-20%PbTiO_3 by scanning force microscopy."Journal of Korean Physical Socciety. 42. S1051-S1054 (2003)
• [Publications] Y.Yoneda, N.Matsumoto, H.Terauchi, N.Yasuda: "Defect-induced phase separation in relaxor PIN."J.Phys.Cond.Matt.. 15. 467-474 (2003)
• [Publications] M.Iwata, K.Katuraya, M.Maeda, I.Suzuki, N.Yasuda, Y.Ishibashi: "Domain observation in PZN-PT mixed crystals by scanning probe microscope."Jpn.J.Appl.Phys.. 42. 5403-5406 (2003)
• [Publications] N.Yasuda, M.Sakaguchi, Y.Itoh, H.Ohwa, Y.Yamashita, M.Iwata, Y.Ishibashi: "Effect of electric field on domain structure and dielectric properties in PIN-PT solid solutions near morphotropic phase boundary."Jpn.J.Appl.Phys.. 42. 6205-6208 (2003)
• [Publications] N.Yasuda, H.Inaba, H.Ohwa, M.Iwata, H.Terauchi, Y.Ishibashi: "Dielectric relaxation in PYN-PT solid solution single crystal near morphotropic phase boundary."Appl.Phys.Lett.. 83. 1409-1410 (2003)
• [Publications] M.Iwata, S.Katagiri, H.Orihara, M.Maeda, I.Suzuki, H.Ohwa, N.Yasuda, Y.Ishibashi: "Annealing Effect of the Phase Transition in PIN crystal."10 th European Ferroelectric Meeting, 2003 August 3-8, Cambridge, England.. 160 (2003)
• [Publications] H.Ohwa, A.Nakada, K.Kaitou, N.Yasuda, M.Iwata, Y.Ishibashi: "Dielectric properties in ACu_3Ti_4O_<12>(A-Ca,Sr,Ba)."10 th European Ferroelectric Meeting, 2003 August 3-8, Cambridge, England.. 245 (2003)
• [Publications] N.Yasuda, N.Uemura, H.Ohwa, M.Iwata, Y.Ishibashi: "Effects of electric field on domain structure and dielectric properties in rhombohedral (001) plate in PMN-PT solid solutions."10 th European Ferroelectric Meeting, 2003 August 3-8, Cambridge, England.. 365 (2003)
• [Publications] N.Yasuda, Y.Itoh, H.Ohwa, Y.Yamashita, M.Iwata, Y.Ishibashi: "Crystal growth of relaxor ferroelectric solid solution single crystal near morphotropic phase boundary with high Curie temperature and some properties."8^<th> Intern.Conf.On IUMRS-ICAM2003.. 212 (2003)
• [Publications] M.Iwata, M.Maeda, I.Suzuki, N.Yasuda, Y.Ishibashi: "Evaluation of domain observation in Pb(Zn_<1/3>Nb_<2/3>)O_3-20%PbTiO_3 by Kelvin force microscopy."8^<th> Intern.Conf.On IUMRS-ICAM2003.. 182 (2003)
• [Publications] D.Ricinschi, Y.Ishibashi, M.Iwata, M.Noda, M.Okuyama: "A Lamdau-Theory-Based Computatinal Study of In-Plane and Out-Plane Polarization Components Role in Switching of Ferooelectric Thin Films."Journal of Korean Physical Socciety. 42. S1232-S1236 (2003)
• [Publications] Y.Ishibashi, M.Iwata: "Phenomenology of Elastic Properties in Martensite Alloys."Journal of the Physical Society of Japan. 72. 1675-1681 (2003)
• [Publications] Y.Gorouya, Y.Tsujimi, M.Iwata, T.Yagi: "Brillouin Scattering Study on Relaxor Ferroelectric Pb(Zn_<1/3>Nb_<2/3>)O_3."Applied Physics Letters. 83. 1358-1360 (2003)
• [Publications] M.Iwata, Y.Ishibashi: "Phenomenology of Elastic Properties in Martensite Alloys II."Journal of the Physical Society of Japan. 72. 2834-2849 (2003)
• [Publications] N.Yasuda et al.: "Dielectirc and piezoelectric properties of lead indium niobate-lead titanate single crystal with high Curie temperature…"Ferroelectircs. 270. 1433 (2002)
• [Publications] M.Iwata et al.: "A Raman scattering study in relaxor mixed crystals Pb(Zn_<1/3>Nb_<2/3>)O_3-PbTiO_3"Ferroelectircs. 270. 1329 (2002)
• [Publications] N.Yasuda et al.: "Crystal growth and some properties of Lead indium niobate lead titanate single crystals produced by solution Bridgman method"Jpn.J.Appl.Phys.. 41. 7007 (2002)
• [Publications] M.Iwata et al.: "Domain observation in PZN-PT mixed crystal"Jpn.J.Appl.Phys.. 41. 7003 (2002)
• [Publications] N.Yasuda et al.: "The relation between polarization and electric field for the phase transition from antiferroelectric to ferroelectric one"J.Korean Phys.Soc.. (in press).
• [Publications] N.Yasuda et al.: "Domain observation in PIN-PT mixed crystal near morphotropic phase boundary"J.Korean Phys.Soc.. (in press).
• [Publications] H.Ohwa et al.: "Pressure effect of dielectric property in solid solutions (1-x)Pb(Mg_<1/3>Nb_<2/3>)O_3-xPbZrO_3"J.Korean Phys.Soc.. (in press).
• [Publications] M.Iwata et al.: "Observation of domain-wall structure in Pb(Zn_<1/3>Nb_<2/3>)O_3-20%PbTiO_3 by scanning force microscopy"J.Korean Phys.Soc.. (in press).
• [Publications] N.Yasuda et al.: "Domain observation in Pb(In_<1/2>Nb_<1/2>)O_3-PbTiO_3 solid solutions near morphotropic phase boundary by polarizing microscope"Transactions of Material Research Society of Japan. 28. 161 (2003)
• [Publications] M.Iwata et al.: "Domain-wall observation in Pb(Zn_<1/3>Nb_<2/3>)O_3-PbTiO_3 solid solutions by AFM"14^<th> symposium of Material Research Society of Japan, Dec.20-21,2002,Tokyo, Japan. (in press).
• [Publications] M.Iwata et al.: "Hetero sturucutre and electro-optic in relaxor Pb(Mg_<1/3>Nb_<2/3>)O_3"Trans.Mat.Res.Soc.Jpn.. 27. 219 (2002)
• [Publications] H.J.Fan et al.: "Brilluan and dielectric studies of the phase transition in the relaxor ferroelectric Pb(Ni_<1/3>Nb_<2/3>)O_3"J.Appl.Phys.. 91. 2262 (2002)
• [Publications] M.Iwata et al.: "Anisotropy of Piezoelectricity near Morphotropic Phase Boundary in Perovskite-Type Oxide Ferroelectrics"Ferroelectrics. 266. 57 (2002)
• [Publications] M.Maeda et al.: "Dielectric Properties of Ethylenediamine Cobalt Nitrate(ECN) Single Crystals"Ferroelectrics. 268. 381 (2002)
• [Publications] Y.Ishibashi et al.: "On an Isomorphous Transition II"J.Phys.Soc.Jpn.. 71. 2576 (2002)
• [Publications] 岩田 真, 石橋善弘: "強誘電体のドメイン"Ferroelectric Domains""機能性材料. 22巻12月号. 5 (2002)
• [Publications] D.Ricinschi et al.: "A Landau-Theory Based Computational Study of In-Plane and Out-Plane Polarization Components Role In Switching"J.Korean Phys.Soc.. (in press).
• [Publications] M.Iwata et al.: "Raman Scattering in the Pb(Zn_<1/3>Nb_<2/3>)O_3-PbTiO_3 Mixed Crystal System II"Jpn. J. Appl. Phys.. 40. 5819-5822 (2001)
• [Publications] M.Iwata et al.: "A Raman Study of Phase Transitions in the Pb(Zn_<1/3>Nb_<2/3>)O_3-PbTiO_3 System"Ferroelectrics. 261. 83-88 (2001)
• [Publications] N.Yasuda et al.: "Crystal growth and dielectric properties of solid solutions of Pb(Yb_<1/2>Nb_<1/2>)O_3 PbTiO_3 with a High Curie Temperature near"Jpn. J. Appl. Phys.. 40. 5664-5667 (2001)
• [Publications] N.Yasuda et al.: "Crystal growth and electrical properties of lead indium niobate-lead titanate binary single crystal"J. Crystal Growth. 229. 229-304 (2001)
• [Publications] H.Ohwa et al.: "Raman Scattering in (1-x)Pb(Mg_<1/3>Nb_<2/3>)O_3-xPbTiO_3"J. Phys. Soc. Jpn.. 70. 3149-3154 (2001)
• [Publications] M.Iwata et al.: "Raman Scattering study in relaxor mixed crystals Pb(Zn_<1/3>Nb_<2/3>)O_3-PbTiO_3"Ferroelectrics. (2002)
• [Publications] N.Yasuda et al.: "Dielectric and Piezoelectric Properties of Lead Indium Niobate-Lead Titanate Single Crystals with High Curie Temperature near Morphotropic Phase"Ferroelectrics. (2002)
• [Publications] N.Yasuda et al.: "On Fatigue and Imprint in Engineered Domain Configurations For Lead-based Complex Perovskite Compounds with High Curie Temperature"1^<st> International Meeting on Ferroelectric Randam Access Memories. FED-175. 103-104 (2001)
• [Publications] N.Yasuda, et al.: "Dielectric Properties of Lead Indium Niobate-Lead Titanate Single Crystals with High Curie Temperature near Morphotropic Phase Boundary"The 8^<th> Workshop on Oxide Electronics. 51 (2001)
• [Publications] H.J.Fan et al.: "Brillouin and dielectric studies of the phase transition in the relaxor ferroelectric Pb(Ni_<1/3>Nb_<2/3>)O_3"J. Appl. Phys.. Vol.91 No.4. 2262-2266 (2002)
• [Publications] Y.Yamashita et al.: "Present and Future of Piezoelectric Single Crystals and the Importance of B-site Cations for High Piezoelectric Response"IEEE Transactions on Ultrasonics, Ferroelectrics, and Frequency Control. Vol.49No.2. 184-192 (2002)
• [Publications] M.Iwata et al.: "Hetero structure and electro-optic effect in relator Pb(Mg_<1/3>Nb_<2/3>)O_3"Trans. Mat. Res. Soc. Jpn.. (2002)
• [Publications] Y.Ishibashi et al.: "On the Lattice Instability in Incommensurate Phase Transition of K_2SeO_4"J. Phys. Soc. Jpn.. 70. 3178-3179 (2001)
• [Publications] M.H.Kuok et al.: "Hypersonic Frequency and Damping Anomalies in Relaxor Ferroelectric Pb(Zn_<1/3>Nb_<2/3>)O_3"Appl. Phys. Let.. 78. 1727-1729 (2001)
• [Publications] M.H.Kuok et al.: "Hypersonic Frequency Softening and relaxation in Relaxor Ferroelectric 0.8Pb(Zn_<1/3>Nb_<2/3>)O_3-0.2PbTiO_3"Solid State Communications. 118. 169-172 (2001)
• [Publications] M.Iwata et al.: "Theory of Morphotropic Phase Boundary in Solid Solution Systems of Perovskite-Type Oxide Ferroelectrics : Engineered Domain Configurations II"Jpn. J. Appl. Phys.. 40. 703-707 (2001)
• [Publications] M.Iwata et al.: "A Theory of Polarization Reversals near the Morphotropic Phase Boundary of Perovskite-Type Oxide Ferroelectrics"Jpn. J. Appl. Phys.. 40. 708-712 (2001)
• [Publications] N.Yasuda et.al.: "Piezoelectric Properties of a High Curie Temperature Pb(In_<1/2>Nb_<1/2>)O_3-PbTiO_3 Binary System Single Crystal near a Morphotoropic Phase Boundary."Jpn.J.Appl.Phys.. 39. L66-L68 (2000)
• [Publications] H.Ohwa et.al.: "Observation of the Distribution of the Transition Temperature in Pb(In_<1/2>Nb_<1/2>)O_3."J.Phys.Soc.Jpn.. 69. 1533-1537 (2000)
• [Publications] N.Yasuda et.al.: "Temperature Dependence of Piezoelectric Propeties of a High Curie Temperature Pb(In_<1/2>Nb_<1/2>)O_3-PbTiO_3 Binary System Single Crystal near a Morphotoropic…."Jpn.J.Appl.Phys.. 39. 5586-5585 (2000)
• [Publications] S.Ishino et.al.: "X-ray Diffraction Study of Domain Reversal in Relaxor Pb(Zn_<1/3>Nb_<2/3>)O_3."J.Phys.Soc.Jpn.. 69. 3154-3157 (2000)
• [Publications] M.Iwata et al.: "Theory of Morphotoropic Phase Boundary in Solid Soltion Systems of Perovskite-type Oxide Ferroelectrics : Engineered Domain Configurations."Jpn.J.Appl.Phys.. 39 No.9A. 5156-5163 (2000)
• [Publications] M.Iwata et.al.: "Raman Scattering in the Pb(Zn_<1/3>Nb_<2/3>)O_3-PbTiO_3 Mixed Crystal System."Jpn.J.Appl.Phys.. 39 No.9B. 5156-5163 (2000)
• [Publications] M.Iwata et al.: "Theory of Morphotoropic Phase Boundary in Solid Solution Systems of Perovskite-type Oxide Ferroelectrics : Engineered Domain Configuration II."Jpn.J.Appl.Phys.. 40 No.2A. (2001)
• [Publications] M.Iwata et.al.: "A Theory of Polarization Reversals near the morphotoropic Phase Boundary of Perovskite-type Oxide Ferroelectrics."Jpn.J.Appl.Phys.. 40 No.2A. (2001)
• [Publications] M.H.Kuok et.al.: "Hypersonic Frequency and Damping Anomalies in Relaxor Ferroelectrics Pb(Zn_<1/3>Nb_<2/3>)O_3."Appl.Phys.Lett..
• [Publications] M.Iwata et.al.: "A Raman Study of Phase Transitions in the Pb(Zn_<1/3>3Nb_<2/3>)O_3-PbTiO_3 System."Ferroelectrics.
• [Publications] M.Iwata et.al.: "A Raman Study of Phase Transitions in the Pb(Zn_<1/3>Nb_<2/3>)O_3-PbTiO_3 System."The 3rd Asian Meeting on Ferroelectricity, Hong Kong, December 12-15,2000. Program book with abstracts. 240
• [Publications] N.Yasuda et.al.: "Crystal Growth and Electrical Properties of Lead Indium Niobate-Lead Titanate Binary Single Crystal."J.Crystal Growth. CGCT-1. 139-140 (2000)