D EPEND ENCE OF D IEL ECTR IC PERM ITTIV ITY ON EL ECTR IC F IELD FOR TH ICK CERAM IC-TY PE FERROEL ECTR IC COM POSITE F ILM S

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1 A CTA M A T ER IA E COM PO S ITA E S IN ICA V o l. 17 N o. 3 A ugust 2000 : (2000) , 2, 2 (1., ; 2.,, ) : PZT gp (VD F2T rfe) PT gp (VD F2T rfe) 023 Υ> 013, Υ< 011, M axw ell2garnett B ruggem an (< 1M V gm ) L z, Yam ada, L z : PZT gp (VD F2T rfe); PT gp (VD F2T rfe); ; ; : TB 333; TM 22 : A D EPEND ENCE OF D IEL ECTR IC PERM ITTIV ITY ON EL ECTR IC F IELD FOR TH ICK CERAM IC-TY PE FERROEL ECTR IC COM POSITE F ILM S ZHAN G X ing2yuan 1, CHAN W ON G L ai2w ah 2, CHO Y Chung2loong 2 (1. D epartm ent of Po lym er Science and Engineering, U niversity of Science and T echno logy of Ch ina, H efei , Ch ina; 2. D epartm ent of A pp lied Physics and M aterials R esearch Centre, T he Hong Kong Po lytechnic U niversity, H ung Hom, Kow loon, Hong Kong, Ch ina) Abstract: M easu ring apparatu s and data p rocessing m ethod of dielectric perm ittivity at h igh vo ltage have been set up. D ependence of dielectric perm ittivity on electric field fo r th ick PZT gp (VD F2T rfe) and PT gp (VD F2T rfe) 023 ferroelectric compo site film s has been investigated. T he dielectric perm ittivity increases obviou sly w ith the increase of app lied field fo r the compo site w ith the vo lum e fraction of ceram ic Υmo re than 013. M axw ell2garnett equation can on ly be u sed to p redict perm ittivity of the compo site w hen Υis less than 011. B ruggem an equation is su itab le fo r the p rediction of dielectric perm ittivity of compo site under low electric field (< 1 M V gm ). Fo r the dep endence of d ielect ric p erm it t ivity on elect ric field, good ag reem en t is found betw een the m easu red perm ittivity and the p rediction of Yam ada model w ith the change of param eter L z, w h ich indicates that L z is determ ined by dim en sion of the componen t, grain shape and static in teraction among the grain s. Key words: PZT gp (VD F2T rfe ) ; PT gp (VD F2T rfe ) ; ferroelectric compo site; dielectric p erm it t ivity; elect ric field dep endence (VD F) 2 (T rfe) 023,, [1 3 ] (PZT ) (PT ) VD F2T rfe PZT gp [VD F ( 77) 2T rfe ( 23) ] PT gp [VD F (70) 2T rfe (30) ] 023,, : ; : : ( ) ; RGC : (1955),,,,

2 64, [4 7 ], F. G. Sh in [8, 9 ] VD F2T rfe, T. Fu rukaw a [10 ] PZT PT VD F2T rfe 023,,, M axw ell2garnett (C lau siu s M o sso ti) [11 ], B ruggem an [12 ] Yam ada [13 ] (M odel 20g20A, T rek Incopo rated) (M odel SR 830, Stanfo rd R esearch System s) 1 kh z + - ( ), PT (3) B 2 PT gp [VD F ( 70) 2T rfe (30) ] M V gm 2 h,, B 1, ( T ek tron ix M odel 2252 ) A B 1 (M odel H P 3589A ),, B 2, kh z (1 10M V gm ) H eiler [14, 15 ], Ε (1) Ε0Ε j 0sin Η = 2Πf 0E 0 V R gr g sin Η 2Πf 0E 0 (1) : Ε0= Fgm ; f 0 ; E 0 ; j 0 ; Η ; V R ; R, - 80 db, 1. 2 VD F (70) 2T rfe (30) VD F (77) 2 T rfe (23) [ mo l % ] P iezo tech Co., PT, PZT ( ),,, 200, (Bueh ler R Isom et TM 2000) 500 Λm ( mm ) ( 100 mm 2 ) PT ; PZT (PK I 522) P iezo K inetics Inc., 1285 PT PZT, 019 Λm 3 : ( 1) A PZT gp [VD F (77) 2T rfe (23) ],, (2) B 1 PT gp [VD F (70) 2T rfe (30) ] M V gm 2 h, 2, (1) Ε PZT gp [VD F (77) 2T rfe (23) ] ( A ), Ε 1, PZT Υ 012, Ε ; Υ 013, Ε, 1 M V gm M V gm 3811 Υ, Ε Υ 015, 1 M V gm 8 M V gm, Ε , 71%, Υ % PT gp [VD F (70) 2T rfe (30) ] Ε A,,, A 2

3 , : 65 B 2 Ε, B 1 PT Υ 013, Ε, Υ 015, Ε, 1 M V gm M V gm 5314, 11%, A B 1 B 2,, B 2,, Υ, Ε B 2 1 PZT gp [VD F (77) 2T rfe (23) ] F ig. 1 Co rrelation of dielectric perm ittivity w ith the intensity of electric field fo r th ick PZT gp [VD F (77) 2T rfe (23) ] film s M axw ell2garnett [11 ] (2) C lau siu s2m o ssitti [16 ] (3) Ε= Εp Εc + 2Εp + 2Υ(Εc - Εp) Εc + 2Εp - Υ(Εc - Εp) Ε- Εp Ε+ 2Εp = Υ Εc - Εp Εc + 2Εp (2) (3) : Εc Εp Ε ; Υ, PZT 2860, VD F (77) gt rfe (23) 1017; VD F (70) gt rfe (30) 1213, 1112; PT 252, 245, Εc Εp Υ, (2) (3) 3 PZT gp [VD F (77) 2T rfe (23) ] Εp = 1017, Εc= 2 860, (2) 3, (2) PZT (Υ< 011), Υ,, PZT, 2 PT gp [VD F (70) 2T rfe (30) ] (B 2) F ig. 2 Co rrelation of dielectric perm ittivity w ith the intensity of electric field fo r th ick PT gp [VD F (70) 2T rfe (30) ] (B 2) film s ( ) ( ), 3 PZT gp [VD F (77) 2T rfe (23) ] F ig. 3 Comparison of the component dependence of dielectric perm ittivity fo r the experim ental and fitting results in PZT gp [VD F (77) 2T rfe (23) ] compo site 4 B 1 PT Ε 4, (2) ( Εp = 1213 Εc= 245) PT Υ 011 Υ 011,, Υ B 2

4 66, ( Εp = 1112 Εc= 245) B 1 3,M axw ell2garnett Υ< 011 PZT PT PT gp [VD F (70) 2T rfe (30) ] (B 1) F ig. 4 Comparison of the component dependence of dielectric perm ittivity fo r the experim ental and fitting results in PT gp [VD F (70) 2T rfe (30) ] (B 1) compo site, B ruggem an (4) [12 ] Ε Ε Ε 1g3 = (1 - Υ) (Εc - Εp ) Εp 1g3 Εc - (4) (4) (2) A B 1 B 2, (4) Ε,, (4) (2) A B 1, B ruggem an 3 4 A B 1 B 2 (4), ( 1 M V gm ), B ruggem an B ruggem an,, B ruggem an, PZT PT, VD F 023,,, 1 4, B ruggem an Yam ada PZT PVD F, ( ) ( ), (5) [13 ] Ε= Εp 1 + Υ(Εc - Εp) Εp + (Εc - Εp) (1 - Υ)L z (5) : Εc Εp Ε Υ (2) ; L z, [13, 16, 17 ] L z = 2 0 abc du (u + c 2 ) (u + a 2 ) (u + b 2 ) (u + c 2 ) (6) : a b c x y z ; z (5) PZT gp [VD F (77) 2T rfe (23) ] PT gp [VD F (70) 2T rfe (30) ], L z, (5) 3 4 Yam ada ( 3 2 1M V gm 8M V gm ; 4 1 M V gm 10 M V gm 2 ), 3 A B 1 B 2 Ε L z, L z, PZT gp [VD F (77) 2T rfe (23) ], L z ; PT PT gp [VD F (70) 2T rfe (30) ], L z ; PT Yam ada, L z, (5) Ε (5) 3 A B 1 B 2 L z 5 5, 3 L z, A ( ) B 1 B 2, L z, (6) x y a b, (6) L z cga cga 0, L z 1; cg a 1,, L z 1g3; cga 10, L z cga,, L z Yam ada PZT gpvd F,

5 , : 67 n= 815 (n L z ), L z = 1gn= [13 ], cga L z, 218, 5 F ig. 5 D epo larization field coefficient decreases w ith the increase of electric field fo r samp le B 1, samp le B 2 and samp le A Yam ada PZT ( SEM ),, 218, ;,,D ias [1 ] Banno [18 ], 1gL z,,,,, L z cga 1 A B 1 B 2,, (6) cga L z, 5 L z, cga A ; B ; B , 023,, ( ) Υ,, (2) (4) Υ,,,,, 3 Υ,, Ε,,,, Ε, Ε Υ 3, Υ , Υ 015 () 4912, Υ,,, Υ Ε B 1 B 2,, Υ,, Ε, 5 A B 1 B 2 L z, Banno,,, L z,, Yam ada 3 ( 1 ) PZT gp (VD F2T rfe ) PT gp (VD F2

6 68 T rfe ) , (2) B ruggem an 1M V gm Yam ada (3) : [ 1 ] D ias C J, D as2gup ta D K. P iezo2 and pyroelectricity in ferroelectric ceram ic2po lym er compo sites[a ]. In: D as2gup ta D K, ed. Ferroelectric Po lym ers and Ceram ic2po lym er Compo sites [C ] Sw itzerland: T rans Tech Publications L td, [ 2 ] Chan H L W, Chen Y, Choy C L. T herm al hysteresis in the perm ittivity and po larization of lead zirconate titanateg vinylidenefluo ride2trifluo roethylene 023 compo sites [ J ]. IE E E T rans D iel E lect Insu l, 1996, 3: [ 3 ] Chan H L W, Guy I L. P iezoelectric ceram icgpo lym er compo sites fo r h igh frequency app lications[a ]. In: D as2gup ta D K, ed. Ferroelectric Po lym ers and Ceram ic2po lym er Compo sites [C ] Sw itzerland: T rans Tech Publications L td, [ 4 ] Rayleigh L. O n the influence of obstacles arranged in rectangular o rder upon the p roperties of a m edium [J ]. M ag, 1892, 32: P h il [ 5 ] W iener O. D ie theo rie des m ischko rpers fur das feld der statona β ren strom ng [J ]. A bh M a th P hy s sach W iess,, 1912, 32: [ 6 ] Kubo M, N akam uro S. D ielectric constant of dispersions of spherical particles[j ]. B ull Chem S oc J p n, 1953, 26: [ 7 ] L andau L D, L ifsch itz E M. E lectrodynam ics of continuous m edia[m ]. O xfo rd: Pergamon P ress, [ 8 ] Sh in F G, T sui W L, Yeung Y Y. D ielectric constant of binary m ixtures[j ]. J M at S ci L ett, 1989, 8: [ 9 ] Sh in F G, Yeung Y Y, T sui W L. Symm etrization of dielectric binary m ixture fo rm ulae [J ]. J M at S ci L ett, 1990, 9: [ 10 ] Furukaw a T. Ferroelectric p roperties of vinylidene fluo ride copo lym ers[j ]. P hase T ransitions, 1989, 18: [ 11 ] M axw ell2garnett J C. Co lours in m etal glasses and in m etal film s[j ]. T ransac R oy S oc, 1904, 203: [ 12 ] B ruggem an D A G. Berechnung versch iedener physikalischer konstanten von heterogenen substanzen [ J ]. A nn P hy s, 1935, 24: [ 13 ] Yam ada T, U eda T, Kitayam a T. P iezoelectricity of a h igh2 content lead zirconate titanategpo lym er compo site[j ]. J A pp l P hy s, 1982, 53: [ 14 ] H eiler B, P lo ss B. D ielectric nonlinearities of P (VD F2 TRFE) [A ]. In: P roc 8th Int Symp on Electrets [C ]. IEEE Inc, Paris: [ 15 ] H eiler B, P lo ss B. D eterm ination of sm all bias fields in T GS using dielectric nonlinearities [ J ]. F erroelectrics, 1994, 156: [ 16 ] SareniB, Kra β henb h l L, Beroual A, B ro sseau C. Effective dielectric constant of periodic compo site m aterials[j ]. J A pp l P hy s, 1996, 80: [ 17 ] P riou A. D ielectric p roperties of heterogeneous m aterials [M ]. N ew Yo rk: Elsevier, [ 18 ] Banno H. T heo retical equations fo r dielectric and p iezoelectric p roperties of ferroelectric compo sites based on modified cubes model[j ]. J p n J A pp l P hy s, 1985, 24 (supp l 2) :

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