Jou rna lo fAd va n c edC e ram i c s 2014 ,3 (3 ) :194– 206 DO I :10 .1007 / s4 0145 -014 -01 10 -4 ISSN2226 -4108 CN10 -1 154 /TQ Re sea r chA r t i c le P repa ra t ion ,c rys ta l l iza t ion ,m ic ros t ruc tu reandd ie lec t r icp rope r t ies o fleadb ismu tht i tana te bo ros i l ica teg lassce ram ics a b Ch andk i r amR .GAUTAMa,*,Abh i sh ek MADHESH IYA ,R an ab r a t a MAZUMDER a Ad va n c e dG l a s sa ndG l a s sC eram i cR e s ea r chL abo ra to r y ,D epa r tm en to fPh y s i c s , Un i v e r s i t yo fLu c know,L u c k now2 26 00 7 ,Ind i a b D epa r tm en to fC eram i cEng in e e r i ng ,N a t ion a lIn s t i tu t eo fT e c hn o l og y ,R o u e r k e l a7 69 00 8 ,I n d i a R e c e iv ed :Ap r i l10 ,2014;R e v i s e d :M a y1 5 ,2 0 1 4 ;A c c e p t e d :M a y2 8 ,2 0 1 4 ©T h eA u t h o r ( s )20 1 4 .T h i sa r t i c l ei spu b l i s h e dw i t hop e na c c e s sa tS p r i ng e r l i nk . c om Ab s t ra c t:V a r iou sb u l kan dt r an s p a r e n tg l a s s e sw e r ep r ep a r e dbyr ap i dm e l tqu e n ch in gt e ch n i qu ein B i1x)T iO – 4 4 [2S iO –L a x=0– 0 .7 ) .Th eX r ayd i f f r a c t io n(XRD ) th eg l a s ssy s t em55 [ (Pb x 3] 2B2O3] 2O3 ( s tud i e so ft h eg l a s ss am p l e scon f i rm edth eam o rpho u sn a tu r e .Th ed i f f e r en t i a lth e rm a la n a ly s e s(DTA ) w e r ec a r r i edou tf romroomt em p e r a tu r eto900℃ w i thah e a t in gr a t eo f10℃/m in .T h eDTAp a t t e rn s o fth es am p l e sshow edo n eo rm o r eexo t h e rm i csh a rpp e a k ssh i f t ingtow a rd slow e rt em p e r a tu r es id e w i thin c r e a s i n gc on c e n t r a t io no fb i sm u thox i d e(B iO ) .Ont h eb a s i so fDTAr e su l t s ,t h eso l idso lu t io n o fb i sm u tht i t anumox id e(B i2T i2O7) / l e a db i sm u tht i t a n iumox id e(Pb i4T i6O21) w a sp r e c i p i t a t edi n 3B bo ro s i l i c a t eg l a s sy m a t r ixa sa m a jo rph a s e .Th eg l a s s e sw e r esub j e c t e dto4han d8hh e a tt r e a tm en t s ch e du l e st oc onv e r tin tog l a s sc e r am i c s . XRDan a l y s i so ft h e s eg l a s sc e r am i cs am p l e sshow e dth a t . 5i sfo un dtoh av e th em a jo rc ry s t a l l in eph a s eo fth ee n t i r eg l a s sc e r am i cs am p l e sw i th0≤ x≤ 0 .7 .T h es c a nn ing cub i cc ry s t a ls t ru c t u r e ,w h i l ei ti st e t r a g on a lfo rg l a s sc e r am i cs am p l ew i t hx=0 i2O7 and e l e c t ron m i c ro s co py (SEM ) m i c rog r a ph si n d i c a t e dth e un i fo rm d i s t r ibu t i o no fB i 2T i4T i6O21 c ry s t a l l i t e sinth eg l a s sy m a t r ix . P b3B Keywo rd s:l e ad b i sm u tht i t a n a t e ;d i f f e r en t i a lth e rm a la n a ly s i s(DTA ) ;c ry s t a l l i z a t i on ;s c a n n in g e l e c t ronm i c ro s copy(SEM ) ;d i e l e c t r i cb e h av i o r 1 In t rodu c t ion F romth el a s tfou rd e c a d e s ,a f t e rt h er em a rk ab l e d i s c ov e ryby Au r iv i l l i u so fan ewf am i lyo fm a t e r i a l s n am ed a f t e rh i sn am e , a co n c e r t ed e f fo r t byth e r e s e a r ch e r sr e su l t e dint h ed i s c ov e ryo fv a r io u sno v e l g l a s sc e r am i c scon t a i n ingf e r ro e l e c t r i cc ry s t a l ssu cha s iT iO a ,K )NbO aT iO b e3O11, B i2WO6, B 3,(N 3, B 3, P 5G i VO5.5, B i eO5, s o l id so lu t i on s o f L iNbO3, B 2 2G a1xT iO3 a n dS rA l i2O8 em b edd e di ng l a s sy P bxB 2S  *Co r r e spond ingau tho r . E -m a i l :g au t am_c e r am i c@ y ahoo . com m a t r ix[1– 1 1 ] . Th em o s tim po r t an ta pp l i c a t i on so f Au r iv i l l i u sf am i ly o fb i sm u th b a s ed f e r ro e l e c t r i c m a t e r i a l sinvo lv e al ay e r e ds t ru c t u r ei nc ap a c i to r s , s en so r s ,a nd p i e zo e l e c t r i cande l e c t ro o p t i cd e v i c e s , wh i ch i ss t r ong ly i n f lu e n c e d by th e m e thod o f p r ep a r a t i on [12–15 ] . Ou to fd i f f e r e n tp r e p a r a t ion m e thod s ,c ry s t a l l i z a t i onf romth eg l a s s e sh a sb e e n app l i e dtosyn th e s i z eth eg l a s sc e r am i c s[16–20 ] .Th i s m e thod g i v e s po s s i b i l i ty o f do p i ng w i th d i f f e r e n t c a t i on stoim p rov eth ep ro p e r t i e so fth eg l a s s e sa nd g l a s sc e r am i c s .I ta l s oa l l ow stoc on t ro lth ep a r t i c l e s i z ee vo lu t i ondu r i ngth et r an s i t io nf romam o r phou s to c ry s t a l l in e s t a t e a n d t o a c h i e v e s u i t ab l e Jou rna lo fAd va n c edC e ram i c s2 014 ,3 (3 ) :194–2 06 c ry s t a l log r aph i co r i e n t a t i o ni n th e po ly c ry s t a l l in e 2 1 ] .S iO2 i si n t ro du c edtoch a ng e th e m a t e r i a l s [ m e l t ingc ond i t ion s ,w h i l e Nd2O3 ad d i t i o nt ob i sm u th t i t a n a t ee f f e c t iv e lyim p rov e sth ee l e c t r i c a lp rop e r t i e s [22–30 ] .Th eg l a s sc e r am i crou t eo fp r ep a r ingB iT iO 3 i sd e s i r ab l etoob t a i nth em a t e r i a la nda s so c i a t e dw i t h po r ef r e ef i n eg r a in so fm i c r o s t ru c tu r eem b ed d e di nth e g l a s s ym a t r ix[2 ] .B e s i d e scon t r o l l i ngt h ec r y s t a l l i t e s i z e ,th i s m e thod a l s op rov i d e st h e con t ro l ov e r th et r a n sp a r e n tc h a r a c t e r i s t i c so ft h ep a r en tg l a s s e s du r i ngth ec r y s t a l l i z a t io n[31 ] .I tw a sr epo r t edth a t g l a s sn ano com po s i t e scom p r i s ing n ano c r y s t a l l i t e so f b i sm u tht i t a n a t e(B iT ) ,d i s p e r s edinag l a s sy m a t r ixo f BO )a c h i e v e dbyt h e s t ron t iumt e t r abo r a t e(S rB 4O7,S con t ro l l e dc ry s t a l l i z a t io no fg l a s s e s [32 ] .I t w a s ob s e rv edth a tu l t r a s on i ct r e a tm en t(UST )o fth eg l a s s s am p l e sw i thanaqu eou ss u sp e n s i ono fB iTfo l l ow ed by conv en t ion a lh e a tt r e a tm en ty i e l d sth ed e s i r e d c ry s t a l l i n eph a s e ,wh i chi so t h e rw i s ed i f f i cu l ttoob t a i n byco nv en t i on a lh e a tt r e a tm en t .G e r t handRü s s e l[18 ] h av er epo r t e dth ec ry s t a l l i z a t ionb eh av io ro fB iTint h e iO –B2O3 sy s t em . How ev e r , th ey h av e B i2O3–T 2 ob s e rv edt h et en d e n cyo fspo n t a n e ou sd ev i t r i f i c a t i on , lys am p l e sw i tht h i c k n e s so fon ly1mmcou l db e andon p rod u c e dw i t hth esy s t embyem p loy in gc o o l i ngr a t ea s h ig ha s22 7℃/m in du r in gc a s t ingo fg l a s sm e l t .Ko j im a e ta l .[16 ]p r e p a r edB iTg l a s sc e r am i c sbyatw in ro l l e r r ap idqu e n c h i ngt e ch n iq u e .R e c en t ly ,t h es tu dyo nth e –S iO2–B i2O3–T iO l a s s e sinth e f ab r i c a t i on o fK 2O 2g s i l i c a t em a t r ixh a sb e e nr epo r t ed .Th eg l a s s e sandt h e i r e r am i c sa r ep r odu c edbyth es im p l ec on v e n t i o n a l g l a s sc m e l t qu e n c h i n gt e ch n i qu efo l low e dbyco n t ro l l e dh e a t r y s t a lc on t a i n in gg l a s s t r e a tm en tto ob t a i nB iT iO 3c c e r am i cn ano com po s i t e sinbu l kq u a n t i t y[3 3 ] .M o r e r e c en t ly ,Go l e z a rd ie ta l .[34 ]r epo r t edth e i r wo rkon c ry s t a l l i z a t ionb e h a v i o r ,m i c ro s t ru c tu r ea ndd i e l e c t r i c p rop e r t i e so fl e adt i t a n a t eg l a s sc e r am i c sint h e sanu c l e a t i ngag en t . p r e s en c eo fB i 2O3 a Th ep r e s e n tp ap e rfo cu s e s onth ec ry s t a l l i z a t i on , m i c ro s t ru c t u r e and d i e l e c t r i cp ro p e r t i e so fg l a s s c e r am i c sw i thv a ry ing B iOco n t e n t .A c co rd in gt oou r know l edg e ,t h e r ei snor e po r tf o rth ep r ep a r a t i ono f g l a s sc e r am i c scon t a in ingt h eph a s e so fso l i ds o lu t i on i2O7) / l e ad b i sm u th o fb i sm u tht i t a num ox id e (B i2T i4T i6O21)by m e l tqu en c h i ng w i th t i t a n i umox id e(Pb 3B a n d L a O , a n d t h e p r e p a r a t i o n , p a r t i c i p a t io no fS iO 2 2 3 c ry s t a l l i z a t io n ,m i c ro s t ru c tu r ean dd i e l e c t r i cb eh a v i o r o ro s i l i c a t eg l a s sc e r am i csy s t emh av e o f(Pb ,B i )T iO 3b no tb e enr epo r t ede l s ew h e r ee i t h e r . 195 2 Ma te r ia l s andme thod s 2 .1 G la s sp repa ra t ion An a ly t i c a lr e ag e n tg r a d e ch em i c a l s PbO (F i sh e r im ed i a , 99 .99% ) , T iO S c i en t i f i c , 99% ) , B i2O3 (H 2 im ed i a , 99 . 5% ) , H3BO3 (H im ed i a , 99% ) ,S iO 2(H O3(H im ed i a ,99 .9% )w e r e (H im e d i a ,9 9 . 8% )a ndL a 2 w e l lm ix edf o r 2hina c e to n em ed i au s in gm o r t a r and p e s t l e . D r i ed powd e r s w e r e m e l t ed i n p l a t in umc ru c ib l efo r1hi nt h et em p e r a tu r er a ng eo f e r no rm a la tm o sph e r i c co nd i t i on 12 00 –1 27 0℃ und d ep en d i ngonth ecom po s i t i on .Th em e l tw a squ en c h e d bypo u r in gi ton t oa na l um inum m ou ldandp r e s s i ng w i that h i cka lum inump l a t e . Th eg l a s s e sw e r eth e n ann e a l eda t400℃ fo r4h . 2 .2 Den s i tymea su remen t s T h ed e n s i tyo fth ep r e p a r e dg l a s s e sa ndg l a s sc e r am i c s am p l e sh a sb e enc a l cu l a t edby A r ch im ed e sp r i n c i p l e [35 ] .D i s t i l l ed w a t e rw a su s eda st h el i qu id m ed ium . Th ed e n s i tyo ft h e s eg l a s s e sandg l a s sc e r am i cs am p l e s i sl i s t edi nT a b l e s1and2 ,r e sp e c t iv e ly .Th efo l low i ng fo rm u l aw a su s edfo rd e t e rm in a t io no ft h ed en s i tyo f g l a s ss am p l e s : W2W1 D e n s i ty ( 1 ) ( W4W1)( W3W2) sth ew e i gh to fem p tysp e c i f i cg r a v i ty wh e r e W1 i bo t t l e(g ) ; W2 i st h ew e igh to fsp e c i f i cg r av i tybo t t l e w i ths am p l e(g ) ; W3 i st h ew e igh to fsp e c i f i cg r a v i ty bo t t l ew i t hs am p l eandd i s t i l l e dw a t e r(g ) ;and W4 i s th ew e i gh to fsp e c i f i cg r av i ty bo t t l ew i th d i s t i l l e d 3 w a t e r(g ) .T h ed e n s i tyo fd i s t i l l edw a t e ri s1 .0g / cm . 2 .3 X‐ rayd i f f ra c t ionmea su remen t s X r ayd i f f r a c t ion(XRD )o fpowd e rg l a s ss am p l e sw a s c a r r i ed ou t u s ing a R ig aku M in i f l ex I I X r ay d i f f r a c t om e t e rw i th C uK r ad i a t iont o ch e ckth e am o rphou ss t a t eo fth ep r e p a r edg l a s ss am p l e s . 2 .4 D i f fe ren t ia ls cann ingca lo r ime t ry mea su remen t s D i f f e r en t i a ls c an n i ng c a l o r im e t ry(DSC )w a s don e u s inga DSCequ ipm en tm od e l NETZSCHSTA449C f romroomt emp e r a tu r e(~27℃)t o90 0℃ em p loy ing ah e a t ing r a t eo f 10℃/m in to d e t e rm in eg l a s s ry s t a l l i z a t ion t r an s i t ion t em p e r a tu r e Tg and c 196 Jou rna lo fAd va n c edC e ram i c s2 014 ,3 (3 ) :194–2 06 T ab l e1 N om en c l a tu r eo fg l a s ss amp l e s , th e i r comp o s i t i on a ld i s t r ibu t i on and g l a s st ran s i t i on t emp e r a tu r e , DTA p e ak and d en s i t y o f v a r i ou s g l a s s samp l e s in th e sy s t em i1x)T iO – 44 [ 2S iO B2O3]–L a 55 [ (PbxB 3] 2 2O3 G l a s ss am p l eco d e x BTL0 .0 PBTL0 .1 PBTL0 .3 PBTL0 .5 PBTL0 .7 0 .0 0 .1 0 .3 0 .5 0 .7 Compo s i t ion(w t% ) S iO a2O3 (P b B i1x)T iO 2–B 2O3 L x 32 55 44 1 55 44 1 55 44 1 55 44 1 55 44 1 C r y s t a l l i z a t ion G l a s st r an s i t ion ℃) t em p e r a tu r eTc( ℃) t em p e r a tu r eTg( 558 626 541 631 532 624 530 622 514 545 ,629 ,770 D e n s i t y 3 ) (g / cm 2 .758 2 .895 3 .009 3 .481 3 .972 T ab l e2 G la s sc e ram i cc od e ,d en s i ty ,h e a t ingr a t e ,hold ingt im e ,ho ld ingt emp e r a tu r e ,c r y s ta ls t ru c tu r e andc r y s t a l l in eph a s e H e a tt r e a tm en ts ch edu l e G l a s sc e r am i c D e n s i t y 3 ) H cod e (g / cm ld ingt im e(h ) Ho e a t ingr a t e(℃/m in ) Ho ld ingt emp e r a tu r e(℃) BTL0 .0626F 2 .765 5 4 626 BTL0 .0626E 2 .785 5 8 626 PBTL0 .1631F 3 .793 5 4 631 PBTL0 .1631E 3 .796 5 8 631 PBTL0 .3624F 3 .864 5 4 624 PBTL0 .3624E 3 .875 5 8 624 PBTL0 .5622F 3 .882 5 4 622 PBTL0 .5622E 3 .888 5 8 622 PBTL0 .7629F 3 .920 5 4 629 PBTL0 .7629E 3 .941 5 8 629 PBTL0 .7770F 3 .963 5 4 770 PBTL0 .7770E 3 .998 5 8 770 BTO—B i2T i2O7(b i sm u tht i t anumox id e ) ;PBTO—Pb i4T i6O21( l e adb i smu tht i t an iumox id e ) . 3B t em p e r a tu r eTc. S in t e r ed a lum in a w a su s ed a sa r e f e r en c em a t e r i a l . Onth eb a s i so fd i f f e r en t i a lth e rm a l an a ly s i s(DTA )r e su l t s ,v a r iou sg l a s sc e r am i cs am p l e s –0 . 5w e r ep r ep a r ed by h e a t w i thc om po s i t ion s x=0 t r e a t ing t h eg l a s s e sin t h et em p e r a tu r er ang eo f o r 4h a nd 8h . Th ed i f f e r en th e a t 62 2– 63 1℃ f t r e a tm en ts c h e du l e san dnom en c l a t u r eo fg l a s sc e r am i c s am p l e sa r el i s t edinT a b l e2 . 2 .5 Nomen c la tu reo fg la s se sandg la s sce ram i c samp le s F iv e l e t t e rg l a s scod e sr e f e rtot h ecom po s i t i ono fth e g l a s s e s .F i r s tt h r e el e t t e r sPBTd e s i gn a t eth ec on t en to f l e a db i sm u tht i t a n a t e .Th ef ou r t hl e t t e rLind i c a t e sth a t O i s u s e d a s a n a d d i t i v e , w h i l e t h e f i f t h 1w t% L a 2 3 l e t t e r ,i . e . ,0 . 0 ,0 .1 ,0 .3 ,0 . 5o r0 .7 ,i nd i c a t e sth ef r a c t i on o fxinth eg l a s ssy s t em .Fo rt h en om en c l a t u r eo fth e g l a s sc e r am i cs am p l e s ,th ef o l l ow in gm e tho do l ogyh a s b e e na do p t ed .F i r s tf iv el et t e r sinth ecod e sfo rth e g l a s sc e r am i cs am p l e sa r es im i l a rtoth ecod e so fth e i r p a r en tg l a s s e sandr e f e rtot h ec om po s i t iono fg l a s s e s , andt h en e x tth r e ed ig i t sind i c a t eth ec r y s t a l l i z a t i on t em p e r a tu r e . Th el a s tl e t t e r Fo r Er e f e r stoth e C r y s t a l s t ru c tu r e Cub i c Cub i c Cub i c Cub i c Cub i c Cub i c Cub i c Cub i c T e t r agon a l T e t r agon a l T e t r agon a l T e t r agon a l C r y s t a l l in e ph a s e BTO BTO BTO BTO BTO BTO BTO BTO PBTO PBTO PBTO PBTO ho l d i ngt im ea tc ry s t a l l i z a t i ont em p e r a tu r e , 4ha nd 8h r e sp e c t iv e ly . T ak e th eg l a s sc e r am i cs am p l e PBTL0 .1631Fa sane x am p l e :th ef i r s tth r e el e t t e r s r ep r e s en tth ec on t en to fl e a db i sm u tht i t a n a t e ,0 . 1 . 1 ) ,6 31i st h e r ep r e s en t st h ev a l u eo fc om po s i t io n( x=0 c ry s t a l l i z a t iont em p e r a tu r e and Fi nd i c a t e sth e 4h so ak ingt im e . Ph a s e sw e r ei d en t i f i ed u s ing powd e r XRD an a ly s i s . D i f f r a c t i on p a t t e rn s w e r er e co rd ed em p loy ingaR ig a k uX r ayd i f f r a c t om e t e ru s in gC uK  r ad i a t i on .T h ec ry s t a l l i n eph a s e sine a c hg l a s sc e r am i c s am p l ew e r eid en t i f i edbyc om p a r ingi t s XRDp a t t e rn w i ths t an d a rdp a t t e rn so fv a r iou sc ry s t a l l in ep h a s e s . 2 .6 Po l i sh ingfo rs cann inge le c t ron m i c ro s copy andd ie le c t r i cmea su remen t s Th eg l a s sc e r am i cs am p l e sw e r eg rou ndan dp o l i s h e d su c c e s s iv e lyu s ing S iCpowd e r sonat h i c ka ndf l a t g l a s sp l a t e .F in a l ly po l i sh i ng w a sc a r r i e do u to na b l a z e rc l o t hu s ingd i am ondp a s t e( 1m ) .Th ep o l i sh e d g l a s sc e r am i cs am p l e sw e r ee t ch edfo r 1m in w i t h + 2 0% H F s o l u t i o n ) . a su i t a b l ee t ch an t (30%HNO 3 E t ch edsu r f a c eo fv a r i ou sg l a s sc e r am i cs am p l e sw a s co a t ed w i t hg o ldbysp u t t e r ing m e thod . Th es am p l e s Jou rna lo fAd va n c edC e ram i c s2 014 ,3 (3 ) :194–2 06 3 Re su l t sandd i s cu s s ion 3 .1 Den s i tymea su remen t ana ly s i s D en s i tyo fa l lth eg l a s s e sandg l a s sc e r am i cs am p l e si s l i s t e di nT ab l e s1a nd2 ,r e sp e c t iv e ly . Asy s t em a t i c t r endi sob s e rv edi nt h ev a lu e so fd en s i t yfo ra l lth e g l a s ss am p l e s .F rom T ab l e1 ,i ti sob s e r v edth a tt h e d en s i tyo fth eg l a s ss am p l e sfo ra l lth ecom po s i t ion s .7 )i n c r e a s e sw i t hi n c r e a s i n gcon c en t r a t i ono f ( x=0–0 3 sm u ch PbO ,b e c a u s eth ed en s i tyo fPb(1 1 . 4g / cm)i 3 ) .Th ed e n s i ty g r e a t e rt h a nt h ed e n s i tyo fB i(9 .8g / cm o fg l a s ss am p l e si sfoundt ol i ei nth er ang eo f 3 / cm. 2 .7 58 –3 . 9 72g Th em e a su r edd en s i tyo fth eg l a s sc e r am i cs am p l e s i sl i s t edinT a b l e2 .I ti sob s e rv edth a tt h ed en s i tyo ft h e g l a s sc e r am i cs am p l e si sfou ndh i gh e rinc om p a r i sonto th ed e n s i ty o f th e i rp a r en tg l a s ss am p l e s . Th i s i s b e c au s e du r i ng t h ec ry s t a l l i z a t io n o r ph a s e t r an s fo rm a t ionch ang ei nvo lum er e su l t s ,i tl e ad stoa ch a ng einth esp e c i f i cg r a v i t y .T h esp e c i f i cg r av i tyo fa g l a s sc e r am i ci so f t end i f f e r en tf romth a to ft h ep a r en t g l a s sb e c a u s eo fsm a l lvo l um ech ang e sth a tm ayo c cu r du r i ngth eh e a tt r e a tm en tp ro c e s s .T h e s ech a ng e sm ay inv o l v ee i th e ras l ig h tc on t r a c t i ono ras l i g h tex p a n s io n , bu ti t wou ldno tu s u a l lyex c e eda3%vo lum ech ang e . H en c e th ec ry s t a l l i n e ph a s e s fo rm ed m ay h av e h ig h e r / low e rd en s i t i e st h a nth eo r i g in a lg l a s s[36 ] . c ry s t a l l i n ep e ak s ,c on f i rm ingal on gr a ng es t r u c t u r a l d i so r d e rc h a r a c t e r i s t i co fam o rph ou sg l a s syn e two rk . 3 .3 D i f fe ren t ia lthe rma lana ly s i s DTAcu rv e so fp r ep a r e dg l as s e sw i thd i f f e r en tl e adto . 7 )a r eshowni nF ig .2 .T h e b i sm u thr a t io s( x=0–0 –0 . 5 DTAp a t t e rn so fg l a s s e sw i thc om po s i t i on s x=0 show on ly on ee xo th e rm i cp e ak . Th e s eexo t h e rm i c p e a k sr e p r e s e n tth et em p e r a tu r ea t wh i c ht h er a t eo f c ry s t a l l i z a t ion o fd i f f e r en t ph a s e si sm ax im um .A l l g l a s s e ssh ow ash i f tint h eb a s el i n ea td i f f e r e n t t em p e r a tu r e s ,d ep e nd in go nth ecom po s i t i on s ,i nt h e t em p e r a tu r er ang eo f514–558℃.Th e s esh i f t si nt h e b a s el i n eshowac h a ng ei nt h esp e c i f i ch e a to fth e g l a s s e s ,w h i c hi sa t t r ibu t e dtoth eg l a s st r an s i t ion 37 –4 0 ] .G l a s st r a n s i t iont em p e r a tu r e s t em p e r a tu r e ,Tg[ o fd i f f e r e n tg l a s ss am p l e sa r eg iv e nin T ab l e1 .T h e g l a s st r a n s i t i ont em p e r a tu r eh a sb e enf oundtod e c r e a s e w i thd e c r e a s i n gco n c e n t r a t io no fB iO .T h i sm ayb ed u e toin c r e a s ei nth ev i s c o s i tyo ft h em e l t .W i thd e c r e a s e inB iOc on t en ti nt h eg l a s ss am p l e s ,t h eg l a s syn e two r k ed u c e s ,an dh en c et h ev i s c o s i tyo f fo rm ingox id eS iO 2r r e th eg l a s s and g l a s st r a n s i t i ont em p e r a tu r eTg a d e c r e a s ed .I ti sr epo r t edbyth ep r e v i ou sr e s e a r ch e r s th a t w i t hd e c r e a s in g co n t en to fn e tw o rk fo rm ing ox i d e s ,th eg l a s st r an s i t io nt em p e r a tu r e sa r er edu c ed . Du et ot h ed e c r e a s eo fn e tw o rk fo rm ingox id e si nt h e g l a s s e sw i thth ead v en to fb i sm u tht i t an a t ei nt h e g l a s s e s ,th ev i s co s i tyandc ro s s l i nk inga r ed e c r e a s ed [1 1 ] .Th e DTAp a t t e rno fth eg l a s ss am p l ePBTL 0 .7 . 7s how st h r e ed i f f e r en tp e ak s w i thcom po s i t ion x=0 (a ) n te s i t a . u . ) II n t e nn s i t yy (( a . u . ) w e r e th en e x am in ed u s i ng a JSM -8 40 s c an n i ng e l e c t ronm i c ro s cop e(SEM )tos tudyth em o rpho l ogyo f d i f f e r en tc ry s t a l l in e ph a s e s . C ap a c i t a n c e (C) and d i s s i p a t io nf a c to r(D) w e r er e co r d eda safun c t iono f ℃ a t t em p e r a tu r eb e tw e enroomt em p e r a tu r ea nd500 z ,1kH z ,1 0kH za nd1MH zu s inga W ayn eK e r r 0 .1kH 65 00 P (h i g hf r equ e n cy LCR m e t e r ,f r equ en cy 20H z –5 MH z ) . Th ev a l u e so fc ap a c i t an c e Ca nd d i s s i p a t io nf a c to rD w e r em e a su r eda safun c t i ono f f r equ e n cya tv a r iou st em p e r a tu r e s . 197 (b ) (c ) 3 .2 X‐ rayd i f f ra c t ionana ly s i so fg la s ssamp le s T r an sp a r en t bu l k a nd t h in g l a s s e s o f op t i c a l B i1x)T iO – qu a l i ty w i t h th e com po s i t i on 55 [ (Pb x 3] 44 [ (2S iO B O ) ] – L a O ( x = 0 – 0 . 7 ) i n m o l a r r a t i o w e r e 2 2 3 2 3 sy n th e s i z e d v i aa c on v en t io n a l m e l t q u en ch in g t e c hn i qu e .A l l XRDp a t t e rn so fv a r i ou sg l a s ss am p l e s BTL0 .0 ,PBTL0 .1 ,PBTL0 .3,PBTL 0 . 5a n dPBTL 0 . 7 a r eshowninF ig .1 .Th e s eXRDp a t t e rn sexh ib i tb ro ad d i f f u s es c a t t e r ing a td i f f e r en t an g l e s in s t e a do f (d ) (e ) 20 30 40 50 60 Twothe e ta ( Deg ree ) 2 θ ( ° ) 70 80 F i g . 1 XRD p a t t e r n so fg l a s ss am p l e sw i t h( a ) ,(b )x=0 .1 ,( c )x=0 . 3 ,(d )x=0 . 5an d( e )x= x=0 0 .7 in th e g l a s s sy s t em 55 [ (P bxB i1x)T iO – 3] –L a . 44 [ 2S iO2B2O3] 2O3 198 Jou rna lo fAd va n c edC e ram i c s2 014 ,3 (3 ) :194–2 06 ( a ) 0 6 2 6℃C 0 5 5 8℃C 0 6 3 1 ℃C ( b ) 0 5 4 1 ℃C XRD p a t t e rn s fo rv a r iou sg l a s sc e r am i cs am p l e s c ry s t a l l i z eda td i f f e r e n tt em p e r a tu r e sw i thah e a t i ng info r4ha r eshowni nF ig .3 .A l lt h e r a t eo f5℃/m p e a k si nr e sp e c t i v e XRDp a t t e rn sa r em a t ch ed w i th 0 6 2 4℃C (888 ) (1153 ) (1244 ) (880 ) (1062 ) (1022 ) (662 ) (800 ) (880 ) (1062 ) (1244 ) (888 ) x=0 .3 (1244 ) (800 ) B i smu tht i tan iumo x ide(B i2T i2O7) Cub i c x=0 .5 Leadb i smu tht i tan iumo x ide(Pb B iT iO ) 3 4 6 21 Te t ragona l (1313 ) (622 ) (0012 ) (0010 ) (e ) x= 0 .7 = 10 20 30 40 50 ° ) 2θ ( (1313 ) (2026 ) ( f ) (1127 ) Leadb i smu tht i tan iumo x ide (Pb B iT iO ) 3 4 6 21 Te t ragona l (0010 ) Tc1,Tc2 andTc3 a tt em p e r a tu r e s545℃,6 29 ℃ a n d nd Tc2 77 0℃, r e sp e c t i v e ly . T h ep e ak sa t Tc1 a a r eob s e rv edexo th e rm i cinn a tu r e wh i l eth ep e a ka t Tc3i sendo th e rm i c(F ig .2 ( e ) ) . Th ep e aka tTc1fo r .5 r e p r e s en t s t h e g l a s s com po s i t io n s x=0–0 c ry s t a l l i z a t io no fth em a jo rb i sm u tht i t an i um ox id e i2O7)ph a s ei na l lt h eg l a s sc e r am i cs am p l e s .Th e (B i 2T . 7(F ig .2 ( e ) ) DTAp a t t e rno fg l a s ss am p l efo r x=0 show sth ep e a ka t5 45℃ du et osom evo l a t i l eim pu r i ty int h eg l a s ss am p l e ,no tdu etot h ec ry s t a l l i z a t i ono ft h e m a jo r /m ino r ph a s e s , wh i l e th ep e a k sa t6 29℃ and 77 0℃ a r e du etot h ec ry s t a l l i z a t ion o ft h e i2O7 (b i sm u th t i t a num ox id e ) /Pb B i4T i6O21 B i2T 3 ( l e ad b i sm u tht i t a n i um ox id e ) ph a s e s . Th i si sa l so con f i rm ed by powd e r XRDs tud i e st h a tth ep e ak s co r r e spondtoth ec ry s t a l l i z a t io no fm a jo rph a s e so fa l l th eg l a s s e s . x 0 . 1 x =0 . 1 (1244 ) (d ) F ig . 2 DTAp a t t e rn so fg l a s ss am p l e sw i th( a ) ,(b ) x=0 . 1 ,( c ) x=0 . 3 ,(d ) x=0 . 5 an d( e ) x=0 x=0 . 7i nt h eg l a s s sy s t em 55 [ (P b B i ) T i O ] x 1x 3– –L a O . 44 [ 2S iO2B2O3] 2 3 (880 ) (1062 ) 9 0 0 (1022 ) 7 5 0 (880 ) (1062 ) 6 0 0 0 (2014 ) 4 5 0 Tem p e r a t u r e( (℃ ) T em p e r a t u r e C ) (800 ) 3 0 0 (444 ) 1 5 0 (800 ) (622 ) 0 7 7 0℃C (1111 ) (1113 ) (200 ) 5 1 4℃C (622 ) 0 B i smu tht i tan iumo x ide(B i2T i2O7) Cub i c (1111 ) (1113 ) ( e ) 0 5 4 5℃C 0 6 2 9℃C (0012 ) x = 0 . 7 x = 0 . 7 In t e n s i t y ( a . u . ) I n t e n s i t y (a .u . ) 5 3 0℃C (1022 ) (c ) B i smu tht i tan iumo x ide(B i2T i2O7) Cub i c 0 (200 ) (b ) (444 ) ( d ) (444 ) 0 6 2 2 ℃C (662 ) 0 5 3 2℃C x = 0 . 5 x= 0 . 5 x= 0 . 0 x = 0 ( c ) (662 ) x = 0 . 3 x = 0 . 3 B i smu tht i tan iumo x ide(B i2T i2O7) Cub i c (622 ) D m T ( a .u . ) T ( V ) (a ) (662 ) x = 0 . 1 x = 0 . 1 3 .4 X‐ rayd i f f ra c t ionana ly s i sand c ry s ta l l i za t ionbehav io r (444 ) x = 0 . 0 x = 0 x=0 .7 60 70 80 F i g . 3 XRD p a t t e r n so fd i f f e r e n tg l a s sc e r am i c s am p l e s :( a ) BTL 0 . 0 62 6F ,(b ) PBTL 0 . 1 6 31F ,( c ) PBTL 0 . 3 6 24F ,(d )PBTL 0 . 5 6 22F ,( e )PBTL 0 . 76 2 9F a nd( f )PBTL 0 . 77 7 0F . Jou rna lo fAd va n c edC e ram i c s2 014 ,3 (3 ) :194–2 06 JCPDS C a rd s No s .3 2 -0 1 1 8a nd35 00 0 7o fv a r i ou s com pound so fcon s t i t u e n to x id e s . XRDp a t t e r nfo rt h e )i sshow nin g l a s sc e r am i cs am p l eBTL 0 .0626F(x=0 F ig .3 ( a ) .I ti sob s e rv edf r omth e XRDp a t t e rnt h a t i2O7, BTO )i st h em a jo r b i sm u tht i t an i umox i d e(B i 2T c ry s t a l l i n eph a s efo rth i sg l a s sc e r am i cs am p l e .F igu r e s 3 (b )an d3 ( c )showth e XRDp a t t e rn so fg l a s sc e r am i c s am p l e s PBTL0 .1 63 1F and PBTL 0 . 36 24F h e a t t r e a t e da td i f f e r en tt em p e r a tu r e s .Th e XRDp a t t e rno f g l a s sc e r am i cs am p l e PBTL0 . 16 31F show st h e i2O7a sa m a jo rph a s e . p r e s en c eo fc ub i cph a s eo fB i 2T Th e XRDd a t ao ft h em a jo rph a s eo fg l a s sc e r am i c –0 . 5 )an dg l a s s s am p l e sr i c hinb i sm u thc o n t e n t( x=0 .7 )a r e c e r am i cs amp l e sr i chi nl e a d con t en t( x=0 i nd e x e do nt h eb a s i so fc u b i ca sw e l la st e t r a g on a lu n i t c e l l s .G l a s sc e r am i ccod e ,d en s i ty ,h e a t i ngr a t e ,ho ld i ng t im e , ho ld i ng t em p e r a tu r e ,c ry s t a ls t ru c tu r e and c ry s t a l l i n e ph a s ea r eg iv e nin T ab l e2 . Th eg l a s s .5 ob t a in e d byth eh e a t c e r am i cs am p l ew i th x=0 t r e a tm en ta t 622 ℃i sfoundt o showth es im i l a r c ry s t a l l i z a t io nb e h a v i o ro fg l a s sc e r am i cs am p l e PBTL0 .3 62 4F(F ig .3 ( c ) ) ,d i f f e r in gs l ig h t ly o n lyi n t e rm so fp e a kin t en s i tya n dv a l u e so f2. T h e XRD p a t t e rn so fg l a s sc e r am i cs am p l e sPBTL 0 .7 62 9Fa nd PBTL0 .7770F a r e shown in F ig s .3 ( e ) and 3 ( f ) , r e sp e c t iv e ly .Th e XRDp a t t e rn so fth e s eg l a s sc e r am i c s am p l e sshowth ep r e s e n c eo ft e t r ag on a lm a jo rph a s e i4T i6O21,PBTO ) . o fl e a db i sm u tht i t an i umox id e(Pb 3B Im p rov edc ry s t an a l i tyh a sb e e nob s e r v e di nth eg l a s s c e r am i cs am p l ew h i c hi sob t a in e dbyh e a tt r e a t inga t 77 0℃ (PBTL0 .7 77 0F )in com pa r i sontoth eg l a s s c e r am i cs am p l eob t a i n e dbyh e a tt r e a t inga t629℃ (PBTL0 .7629F ) . Th ec ry s t a l l i t es i z ew a sc a l cu l a t ed u s in gS c h e r e rfo rm u l a[41 ] : K ( 2 ) Dp  s co  wh e r eKi st h esh a p ef a c to r(0 .94 ) ;i st h ew av e l en g t h o fCu Kαl i n e( 1 . 5 4Å ) ;a n d i sth efu l lw id tha th a l f m ax im um . G l a s sc e r am i cs am p l ec od e ,a v e r a g e c ry s t a l l i t ean dg r a i ns i z eh a v eb e e nl i s t edinT a b l e3 . Th em in im umand m ax im umv a lu e so fc r y s t a l l i t es i z e co r r e sp on d in gt om ax im umin t en s i typ e ak so fg l a s s c e r am i cs am p l e s PBTL0 . 76 29F an d PBTL0 .5 62 2E h av eb e e nfo un d1 .1 0nman d6 6 . 09nm ,andt h e i r av e r a g ec ry s t a l l i t es i z ea r e 83 3nm and 50 0nm , r e sp e c t iv e ly . Th e XRD p a t t e r n s fo rg l a s sc e r am i cs am p l e s BTL0 .0626E , PBTL0 .1631E , PBTL0 .3624E , PBTL0 .5622E ,PBTL0 .7629Ean dPBTL0 .7 77 0Ea r e 199 T ab l e3 G la s sc e ram i cs amp l ecod e ,av e rag e c r y s t a l l i t eandg r a ins i z e G l a s sc e r am i cs am p l e cod e BTL0 .0626F BTL0 .0626E PBTL0 .1631F PBTL0 .1631E PBTL0 .3624F PBTL0 .3624E PBTL0 .5622F PBTL0 .5622E PBTL0 .7629F PBTL0 .7629E PBTL0 .7770F PBTL0 .7770E C r y s t a l l i t es i z e ( nm ) 43 .48 38 .01 50 .75 60 .93 30 .43 27 .67 50 .75 66 .09 1 .10 1 .25 2 .51 2 .87 G r a ins i z e ( nm ) 1250 600 1250 500 500 750 1000 500 833 1250 1250 1250 showninF ig .4 .G l a s sc e r am i cs am p l e s BTL0 . 06 26E andPBTL 0 .1631Eh a v eth eph a s econ s t i tu t ions im i l a r to BTL 0 .0 62 6F a nd PBTL0 .1 63 1F t h a to b t a i n ed by h e a tt r e a t ing fo r 4h . Fo r th eg l a s sc e r am i c s am p l e PBTL0 .3 62 4E ,ac h an g ei s ob s e rv edint h e c ry s t a l l i n en a tu r einth e XRD p a t t e rn o ft h i sg l a s s c e r am i cs am p l ei ncom p a r i sont ot h eg l a s sc e r am i c s am p l ePBTL0 .3 62 4F .Th i sch a ng em ayb edu etob a c k g rou ndno i s eandan ewp e a kob s e rv e da t2 v a l u e 14 . 8 ° co r r e s po nd i ng to th ep l a n e (2 22 ) .S im i l a r c ry s t a l l i z a t io nb e h av io rh a sb e e nob s e r v edfo rg l a s s c e r am i cs am p l ePBTL 0 . 5622E(F ig .4 ( d ) ) . Th em a jo r i4T i6O21, ph a s eo fl e a db i sm u tht i t a n iumox i d e(Pb3B PBTO )i sc ry s t a l l i z edf o rt h eg l a s ss am p l eh e a tt r e a t e d o r8h .Fu r th e r ,f o rth es am eg l a s ss am p l e a t629℃ f c ry s t a l l i z eda t770℃ fo r8hh e a tt r e a tm en ts c h e du l e , th em a jo r ph a s eo f PBTOc ry s t a l l i z e ssu c c e s s fu l ly ; on lyas l ig h tch a ng eh a sb e eno b s e rv e dint h e XRD p a t t e rn o ft h i sg l a s sc e r am i cs am p l ei n wh i c h b ro a dn e s s o f th e p e ak d e c r e a s e s show in g th e d e c r em en tinth e am o rphou sn a t u r eo fth eg l a s s c e r am i cs amp l e . Th e XRD p a t t e rn so fth e s eg l a s s c e r am i cs am p l e sc ry s t a l l i z edfo r4ha sw e l la s8hh e a t t r e a tm en ts ch e du l e sa lo ngw i thSEM m i c rog r a ph sg i v e ad e qu a t ei n fo rm a t ion a b ou tt h e m o rph o lo gy a nd c ry s t a l l i t e ss i z e . 3 .5 Su r fa cemo rpho log i ca l ana ly s i s Th esu r f a c em o rpho l ogyo fa l lg l a s sc e r am i cs am p l e s show sf i n ec r y s t a l l i t e so fm a jo r ph a s e so fb i sm u th i2O7, BTO ) an dl e a db i sm u th t i t a num ox id e (B i 2T i4T i6O21, PBTO ) . Qu a l i t a t i v e t i t a n i um ox i d e (Pb 3B in sp e c t iono fa l lth e s eSEMm i c rog r aph sr ev e a l st h a t th er e l a t i v ec o n t e n to fr e s i du a lg l a s sph a s ei sp r e s en tin (1111 ) (1113 ) (1244 ) (1022 ) (888 ) (1244 ) (888 ) (1062 ) (880 ) (1022 ) (888 ) (1244 ) (880 ) (1062 ) (1022 ) (662 ) (800 ) (1244 ) (888 ) B i smu tht i tan iumo x ide(B i2T i2O7) x = 0 . 5 = 0 . 5 Cub i c (880 ) (1062 ) (622 ) (1111 ) (1113 ) (1313 ) (e ) (2026 ) (2014 ) Leadb i smu tht i tan iumox ide(Pb B iT iO ) 3 4 6 21 Te t ragona l (1127 ) (d ) x = 0 . 1 = 0 . 1 i2O7) B i smu tht i tan iumo x ide(B i2T x= = 0 .3 Cub i c (800 ) (662 ) (444 ) (622 ) (222 ) (880 ) (1062 ) (1153 ) (800 ) (662 ) (800 ) (444 ) (622 ) B i smu tht i tan iumo x ide(B i2T i2O7) Cub i c (c ) (222 ) In t e n s i t y a . . ) I n t e n s i t y (( a . u . )u x= 0 . 0 x = 0 B i smu tht i tan iumox ide(B i2T i2O7) Cub i c (662 ) (b ) (622 ) (a ) (444 ) Jou rna lo fAd va n c edC e ram i c s2 014 ,3 (3 ) :194–2 06 (444 ) 200 x =0 .7 x 10 20 30 40 50 ° ) 2θ ( T th t (D (1313 ) (2026 ) ( f ) (1127 ) (2014 ) (0010 ) (0012 ) (200 ) Leadb i smu tht i tan iumox ide(Pb B iT iO ) 3 4 6 21 Te t ragona l 60 x=0 .7 70 80 ) F i g . 4 XRD p a t t e r n so fd i f f e r e n tg l a s sc e r am i c s am p l e s :( a ) BTL 0 . 0 6 2 6E ,( b ) PBTL0 . 1 6 3 1E ,( c ) PBTL 0 . 3 6 24E ,( d )PBTL 0 . 5 62 2E ,( e )PBTL 0 . 7 62 9E a nd( f )PBTL 0 . 77 7 0E . l i t t l eam oun to rab s en ts ig n i f i c an t lyi nb i sm u thr i ch g l a s sc e r am i cs am p l e s .Th eco e x i s t en c eo fco a r s eand fin ep a r t i c l e sh a sb e ena l s oo b s e rv e dina l lt h eg l a s s c e r am i cs am p l em i c rog r aph ss im i l a rtot h el e a dt i t a n a t e b a s e dg l a s s – c e r am i c s[42 , 4 3 ] .T h eSEM m i c rog r ap h s o fv a r i ou sg l a s sc e r am i cs am p l e sh e a tt r e a t e dfo r4h and8ha r es howni nF i g s .5 –7 .F ig u r e5sh ow sSEM m i c rog r aph so fg l a s sc e r am i cs am p l e s BTL0 . 06 26F , PBTL0 .1 63 1F , PBTL0 . 36 24F , PBTL0 . 56 22F , PBTL0 .7 62 9Fand PBTL0 . 77 70F .T h eg l a s sc e r am i c s am p l e BTL 0 .0 62 6Fi sfou ndt ob e com po s ed o f in t e r co nn e c t e df in ean dun i fo rmc ry s t a l l i t e so fb i sm u th i2O7,BTO ) ,wh i cha r ed i s p e r s edin t i t a numox id e(B i 2T th eg l a s sy m a t r ixa nds ep a r a t e d by w e l ld e v e l op ed g r a inbo un d a r i e sth r ou gh ou tth em i c rog r aph(F ig .5 ( a ) ) . XRDs tud i e scon f i rmth a tt h ef in ec ry s t a l l i t e sa r eBTO wh i chi st h em a jo rc ry s t a l l in eph a s e .Ing e n e r a l ,t h e wh i t er e g i onint h e m i c r o s t ru c t u r er e p r e s en t sth e agg lom e r a t ed m a jo rc ry s t a l l i n eph a s eo f BTO , wh i l e th eb l a c kr eg i ond e p i c t sth er e s id u a lg l a s sina l lSEM m i c rog r aph s . Fo r th e g l a s s c e r am i c s am p l e PBTL0 .1 63 1F ,t h e r ei sac h ang eint h em o rph o l ogyo f th ec ry s t a l l i t e so fth em a jo rph a s e BTO(F ig .5 (b ) ) . Th e s ec ry s t a l l i t e sa r ef oundtoh av ei r r egu l a rsh a p ea nd no tun i fo rm lyd i s t r i bu t e dinth eg l a s sy m a t r ix .F ig u r e 5 ( c )sh ow st h eSEM m i c rog r apho ft h eg l a s sc e r am i c s am p l e PBTL 0 .3624F .T h ec ry s t a l l i t es i z eh a sb e e n foun dinth eo rd e ro fs u b -m i c ronr a n g e , wh i l eth e vo l um ef r a c t iono ft h er e s i du a lg l a s sh a sb e e nfo un d l a r g e .T h ec ry s t a lg row t han dt h e i rd i s t r i b u t i ona r en o t app e a r i ng p r op e r lyint h i sm i c rog r ap h .F ig u r e5 (d ) r ep r e s en t st h eSEM m i c rog r aphfo rth eg l a s sc e r am i c s am p l e PBTL0 .5622F . Th eg l a s sc e r am i cs am p l e PBTL0 .5622Fshow sth ec abbag e l ik ec r y s t a l l i t e sa r e un i f o rm lyd i sp e r s eda sa m a jo rph a s eo f BTOa lo n g w i tht r a c eam oun to fs e c on d a ryph a s eint h eg l a s sy m a t r ix . F igu r e s5 ( e )and5 ( f )d ep ic tth eSEM m i c rog r aph s fo rth eg l a s sc e r am i cs am p l e s PBTL 0 .7629F a nd PBTL0 .7 77 0F ,r e sp e c t i v e ly .T e t r a go n a ll e adb i sm u th B i4T i6O21)i sc ry s t a l l i z e da st h e t i t a n i um ox id e(Pb 3 m a jo rph a s efo rth e s eg l a s sc e r am i cs am p l e s .Th e r ea r e two typ e s o f ph a s ef o rm a t ion s e en in th e s e m i c rog r aph s :( i )t e t r agon a lc ry s t a l l i t e swh i cha r eb igi n .7 ) sh ap eands i z edu et ot h el a r g ec on t en to fPbO( x=0 and( i i )n e e d l e l ik es e c ond a r yph a s edu et oth ec ry s t a l g row tho fth eb i sm u thox id e . Wh enth es am eg l a s s s am p l ei sc ry s t a l l i z e da th i gh e rt em p e r a tu r e770℃,a s l ig h tc h a ng einth em o rph o lo gyh a sb e e nfou ndt h a t th en e ed l e l i k es e c ond a ryph a s ei sob s e rv edv e ryl e s s . F igu r e6sh ow sth eSEM m i c rog r aph so fd i f f e r en t g l a s sc e r am i cs am p l e s BTL0 .0 62 6E , PBTL0 . 16 31E , PBTL0 .3 62 4E an d PBTL0 .3 62 4E ( a t low e r m agn i f i c a t i on ) . Th e s eg l a s sc e r am i cs am p l e sa r e ob t a i n edth r o ug hc ry s t a l l i z a t i ono fth e i rp a r en tg l a s s e s fo r8hh e a tt r e a tm en ts ch e d u l e .Th een t i r em o rpho l ogy Jou rna lo fAd va n c edC e ram i c s2 014 ,3 (3 ) :194–2 06 201 ( a ) (b ) ( c ) (d ) ( e ) ( f ) F i g .5 SEMm i c rog r a p h so fg l a s sc e r am i cs am p l e s :( a )BTL 0 . 0 62 6F ,( b )PBTL 0 . 1 63 1F ,( c )PBTL 0 . 3 6 24F , (d )PBTL 0 . 5 6 2 2F ,( e )PBTL 0 . 76 2 9Fa n d( f )PBTL 0 . 7 7 70F . h a sb e e nfou n dt ob ec h an g edi nc om p a r i sont oth e4h h e a tt r e a t ed g l a s sc e r am i cs am p l e sw i t ht h es am e com po s i t ion s , wh i cha r eno tc l e a rf rom XRDs tud i e s . F igu r e s6 ( a )and 6 (b )d e p ic tt h e SEM m i c rog r aph s o f th eg l a s sc e r am i cs a m p l e s BTL0 .06 26E an d PBTL0 .1631E .T h em o rpho logy o fth ec r y s t a l l i t e si s foun ds im i l a r ,b u tt h eya r ed i f f e r ingint e rm so ft h e c r y s t a lg r ow t ha n dt h e i rd i s t r i b u t i o n . T h e w e l l d ev e l op e d ,in t e r con n e c t e da ndd en s ec ry s t a l l i t e so fth e m a jo rph a s eo f BTOa r ed i sp e r s edun i f o rm lyinth e g l a s sy m a t r ix , wh i l eth ec r y s t a lg row t hfo rth eg l a s s . 1 )a r e no t c e r am i cs am p l e PBTL0 .1631E ( x=0 w e l l d e v e l o p ed a nd t h e a gg lom e r a t io n o f th e c ry s t a l l i t e sa r ea l soob s e rv e d .F ig u r e s6 ( c )an d6 (d ) showt h em i c rog r a ph so fth eg l a s sc e r am i cs am p l e PBTL0 .3 62 4Ea td i f f e r e n tm agn i f i c a t i on s .V e rysh a rp andf i n en e ed l e l i k ec ry s t a lg row t ho fm a jo rp h a s eo f BTOh a sb e e nob s e r v e da l on gw i ths e c on d a ryp h a s e . Wh en w et a k eth e m i c rog r ap ho ft h es am eg l a s s c e r am i cs am p l ePBTL0 .3624Ea tlow e rm agn i f i c a t i on , th es e cond a ryph a s ei sc l e a r lys e eni nd i f f e r en tsh ap e ands i z e . 202 Jou rna lo fAd va n c edC e ram i c s2 014 ,3 (3 ) :194–2 06 ( a ) (b ) ( c ) (d ) F i g . 6 SEM m i c rog r a p h so fg l a s sc e r am i cs am p l e s :( a ) BTL0 . 0 62 6E , (b ) PBTL 0 .1 63 1E , ( c )PBTL 0 . 36 2 4Ea n d( d )PBTL0 . 3 62 4E( a tl ow e rm a gn i f i c a t i on ) . F igu r e7s how sth eSEMo fg l a s sc e r am i cs am p l e s PBTL0 .5 62 2E , PBTL0 . 76 29E , an d PBTL0 .7 70E r e sp e c t iv e ly .F igu r e7 ( a )r e p r e s en t st h em i c rog r apho f th eg l a s sc e r am i cs am p l e PBTL0 . 5622E wh i chi s ob t a i n edby8hh e a tt r e a tm en ts ch ed u l eo fth es am e p a r en tg l a s ss am p l e .V e ryf i n ec ry s t a lg row thh a sb e en ob s e rv eda l on gw i t hn e ed l e l ik es e c on d a ryph a s e .I f w ecom p a r eth i sm i c rog r aphw i th4hh e a tt r e a t edg l a s s c e r am i cs am p l e(F ig .5 (d ) ) ,th eg r a inbound a rys e em s tob ed i s app e a r inga ndin t e r conn e c t e dtoe a cho th e rfo r 8hh e a tt r e a t e dg l a s sc e r am i cs am p l e .F i g u r e s7 ( c )a nd 7 (d )sh owth es im i l a rm o rpho l ogyo fth eg l a s sc e r am i c . s am p l e sh e a tt r e a t e dfo r4h 3 .6 D ie le c t r i cbehav io r n dd i s s i p a t i onf a c t o rD w e r e D i e l e c t r i cc o n s t a n t ra m e a su r ed a s af un c t i on o ft em p e r a tu r ew i t h i nth e ℃ a tv a r iou ss e l e c t e d t em p e r a tu r er ang eo f 50–320 f r equ e n c i e ss u cha s2 0H zto1 .0MH zfo rt en t a t iv e g l a s s c e r am i c s am p l e s PBTL0 .3624F and nd PBTL0 .5 62 2F .F igu r e8s how sth ev a r i a t i on so f ra D w i th t em p e r a tu r ef o r g l a s sc e r am i cs am p l e a sb e enfo un d PBTL0 .3 62 4F .In i t i a l ly ,t h ev a l u eo f rh con s t an tupt oac e r t a inv a lu eo ft em p e r a tu r e200℃, andth e r e a f t e r ,i ti n c r e a s e sw i thin c r e a s i ngt em p e r a tu r e a tl owf r e q u e n c yr a n g ef r om2 0H zt o1kH z ,w h i l et h e sfoun dc on s t an tm e an ingt em p e r a tu r e v a l u eo f ri ind ep en d en ta tt h eh i ghf r equ e n cyr a ng e .Th ev a lu eo f nd d i s s i p a t i onf a c to r Da t d i e l e c t r i c con s t an t ra t em p e r a tu r e60 ℃ a t1kH zh av eb e enfo un dtob e3 2 and0 . 00 13 ,r e sp e c t i v e ly .A lm o s ts im i l a rb eh av io rh a s b e e nob s e rv e dfo rt h ep lo to fd i s s ip a t i o nf a c to rD v s . t em p e r a tu r e .Th em ax im umv a lu eo fd i e l e c t r i ccon s t a n t i sf ou ndt ob et h eo r d e ro f50 0a l o ng w i t hd i s s i p a t i o n f a c to rv a l u e1 . 2 . n d F igu r e9sh ow sth ep lo t so fd i e l e c t r i cc o n s t a n t ra d i s s i p a t io nf a c to rD v s .t em p e r a tu r ef o rth eg l a s s c e r am i cs amp l e PBTL0 . 5622F . Bo thth ep lo t sh a s a n d D , w h i c h m a y b e s im i l a rt r end sandi n c r e a s ein r du et oi n c r e a s ei nth ee l e c t r i c a lc ondu c t i on w i th in c r e a s ingt em p e r a tu r e[44 ] . Th ed i e l e c t r i cb e h a v io ro f th i sg l a s sc e r am i cs am p l ec anb ee xp l a i n edi nt e rm s i ch p r om o t e s th e o f th ea dd i t ion o f L a2O3 wh c ry s t a l l i z a t iono fth eg l a s sdu r i ngt h eh e a tt r e a tm en t . A sm a l lc o n c e n t r a t i on o fd on o rd op a n tL a3+in p e ro v sk i t ec e r am i c si s kn ownt oi nd u c ea nn ty p e Jou rna lo fAd va n c edC e ram i c s2 014 ,3 (3 ) :194–2 06 203 ( a ) (b ) ( c ) F i g . 7 SEM m i c rog r a ph so fg l a s sc e r am i cs am p l e s :( a ) PBTL 0 . 56 22E ,( b ) PBTL0 . 7 62 9Ean d( c ) PBTL 0 . 7 7 0E . s em i cond u c t iv i tybye l e c t ron i cc om p en s a t i on . L a  L a+ e 3+ B iT iO3  S r ( 3 ) Du etoth ed i f f e r en c ei n condu c t iv i t y ,in t e r f a c i a l po l a r i z a t i on a r i s e sa tc r y s t a l–g l a s si n t e r f a c e and a t t r i bu t e st oh ighv a lu eo fd i e l e c t r i ccon s t an t r.Th i s w i t h t h e o r d e r o f 1 1 0 0 c au s e st h ee f f e c t i v ev a l u eo f r [45 ] .T h ein c r e a s ei nth ev a lu eo fd i e l e c t r i ccon s t a n t w i thin c r e a s i ngt em p e r a tu r ea t0 . 1kH zto1kH zf o r th e s eg l a s sc e r am i cs am p l e s m igh tb e du et oth e 2+ in c r e a s ingcon c e n t r a t iono fB ii nt h ep a r e n tg l a s s com po s i t ion s . Th ed i e l e c t r i ccon s t an ta sw e l la sl o s s d a t as how sth a tw i thi n c r e a s ingv a l u eo fx( c on t en to f n dl o s sv a lu e sa r ei n c r e a s e d PbO )int h eg l a s s e s , ra g r adu a l ly .Th i sin c r e a s ein a n d D v a l u e s i s a t t r i b u t e d r toth ee xp end ingcon c e n t r a t i ono fa l k a l ii onc h a r g e c a r r i e r sw i thin c r e a s eo fP bOc on t en tint h eg l a s sin exp en s eo fS iO l e c t r i c a lp rop e r ty o fa g l a s si s 2. E p r im a r i ly con t ro l l e d by th e conn e c t i v i ty o ft h e con t i nuou sg l a s sy ph a s e , andth i sg l a s s ph a s ei s r edu c edandc r y s t a l l in eph a s e sa r ei n c r e a s eda f t e rh e a t t r e a tm en t .I ti s ob s e rv e dt h a tg l a s sc e r am i cs am p l e PBTL0 .5622Fcon t a in sl e s sc ry s t a lc om p a r edtoth e g l a s sc e r am i cs am p l ePBTL0 .3624F ,andi t sd i e l e c t r i c lo s si sm o r ec om p a r edtoPBTL0 . 5622F . Mu rug ane ta l . [2 ]h av ea l s o ob s e rv e dt h a tth ed i e l e c t r i clo s sD d e c r e a s e sw i t hi n c r e a s ingf e r ro e l e c t r i cph a s e si nt h e g l a s s – c e r am i c s ,andt h eya l sor epo r t edth a tD v a lu ei s l e s s fo rg l a s s e s com p a r ed to th e po ly c ry s t a l l i n e c e r am i c sinth es am esy s t em . 4 Con c lu s ion s DTAp a t t e rn so fth eB ir i c hg l a s ss am p l e sshowon ly s ing l eexo t h e rm i cp e a k , wh i l e DTAp a t t e r n so ft h ePb r i chg l a s ss am p l e sshow m o r eth anon eexo t h e rm i c p e a ka sw e l la son eendo th e rm i cp e ak .DTAp e aka tTc fo ra l lg l a s ss am p l e ssh i f t stow a rd slow e rt em p e r a tu r e s id e du et oth ed i f f e r en t m e l t ingt em p e r a t u r e and v i s c o s i tyo ft h em e l t s . Th e XRDp a t t e r n so fB ir i c h g l a s sc e r am i cs am p l e s showth e m a jo r ph a s eo f T i O ) , w h i l e i t i s o b s e r v e d b i sm u tht i t a numox id e(B i 2 2 7 fo r Pbr i ch g l a s sc e r am i cs am p l e sa sl e a db i sm u th B i T i O ) . C r y s t a l l i n e p h a s e o f a l l t i t a n i umox id e(Pb 3 4 6 21 ≤ x≤ 0 .5i sfo un dto th eg l a s sc e r am i cs am p l e sw i th0 . 7i ti s h av e cub i cc r y s t a ls t ru c t u r e , andfo r x=0 ob s e rv edt e t r a gon a lc ry s t a ls t ru c t u r e .Th ee f f e c to fh e a t 204 Jou rna lo fAd va n c edC e ram i c s2 014 ,3 (3 ) :194–2 06 Re la t i v e d i e l e c t r i c c o n s t an t R e l a t i v e d i e l e c t r i cc o n s t a n t Re la t i ved ie lec t r i ccons tan t 500 400 300 200 100 0 60 2 .0 D is s i p a t i o n f a c to r D i s s i p a t i o n fa c t o r 1 .6 1 .4 1 .2 1 .0 0 .8 0 .6 180 240 A cknow ledgemen t s 300 Tempe ra tu re(℃) (b ) 0 .4 0 .2 0 .0 60 120 180 Tempe ra tu re(℃) 240 R e l a t i ve d i e l e c t r i ccon s t a n t Re l a t i v e d i e l e c t r i c n s t a n t 1200 1000 800 600 400 200 0 100 Re fe ren ce s 200 250 300 Tempe ra tu re(℃) 4 3 2 1 0 100 350 400 (b ) 20H z 50H z 100H z 200H z 500H z 1kH z 5kH z 10kH z 30kH z 50kH z 100kH z 300kH z 500kH z 1 MH z 3 MH z 5 MH z 150 OpenA c ce s s:T h i sa r t i c l ei sd i s t r i bu t e du n d e rt h et e rm s o ft h eC r e a t i v eC omm on sA t t r i b u t i o nL i c e n s ew h i c h p e rm i t sanyu s e ,d i s t r i bu t i o n ,a ndr e p r od u c t i oni na ny m e d i um ,p ro v i d edt h eo r i g i n a lau t h o r ( s )an dt h eso u r c e a r ec r e d i t ed . (a ) 20H z 50H z 100H z 200H z 500H z 1kH z 5kH z 10kH z 30kH z 50kH z 100kH z 300kH z 500kH z 1 MH z 3 MH z 5 MH z 150 Th ea u tho r sa r eg r a t e fu l lya cknow l edg edtoth eU t t a r P r ad e shC oun c i lo fS c i e n c eandT e c hno l o gy ,Lu cknow ( Ind i a )fo rf i n an c i a lsu pp o r tu nd e rt h e“Y oun gS c i en t i s t S ch em e ”a sm a jo rr e s e a r chp ro j e c t No .CSTT /YSS /D 39 13 . Au t ho r sa r ea l s ot h a nk fu lto D r .A tu lK h an n a , a s so c i a t ep r o f e s so r ,fo rh i sco n s t an tsu p po r ta ndto ex t end ing th eXRDm e a su r em en tf a c i l i tya tD ep a r tm en t o f Phy s i c s , Gu ru N an a kD ev Un iv e r s i ty , Am r i t s a r 14 30 05 ,Ind i a . 300 F ig .8 V a r i a t ion so f( a )d i e l e c t r i ccon s t an t r and(b )d i s s i p a t i onf a c t o rD w i tht em p e r a tu r ea t d i f f e r e n tf r e qu en c i e s fo rt h eg l a s sc e r am i c s am p l ePBTL0 .3624F . D iss ipa t ionfac to r D iss ipa t ionfac to r D i ss ipa t ionfac to r 120 20H z 50H z 100H z 200H z 500H z 1kH z 5kH z 10kH z 30kH z 50kH z 100kH z 300kH z 500kH z 1 MH z 3 MH z 5 MH z 1 .8 t r e a tm en ts ch edu l efo r4 hand8hc h a ng e sth es u r f a c e m o rpho l ogyo fth ec ry s t a l l i t e s .XRDr e s u l t sr ev e a lth a t e a tt r e a tm en ts ch edu l e sa r efoundt ob eth es am e th eh fo r4ha nd8h .I ti sa l soc on c lu d e dt h a tth ev a l u eo f d i e l e c t r i ccon s t an ti sf oundl a r g e rfo rg l a s sc e r am i c s am p l e PBTL0 .5622Fi n com p a r i sontoth eg l a s s c e r am i cs am p l ePBTL0 .3624F . (a ) 20H z 50H z 100H z 200H z 500H z 1kH z 5kH z 10kH z 30kH z 50kH z 100kH z 300kH z 500kH z 1 MH z 3 MH z 5 MH z 200 250 300 350 400 Tempe ra tu re(℃) F ig .9 V a r i a t ion so f( a )d i e l e c t r i ccon s t an t r and(b )d i s s i p a t i onf a c t o rD w i tht em p e r a tu r ea t d i f f e r e n tf r e qu en c i e s fo rt h eg l a s sc e r am i c s am p l ePBTL0 .5622F . [1 ]A u r i v i l l i u sB . M i x e db i sm u t ho x i d e sw i t hl a y e r T i3O12.A r k i vfo rK em i l a t t i c e s .I I .S t r u c t u r eo fB i 4 19 4 9 ,1:49 9 –5 12 . [2 ]M u r ug a n GS , Su b b an n a GN , V a rm a KBR . N a n o c r y s t a l l i z a t i on o f f e r r o e l e c t r i c s b i sm u t h t un g s t a t ei nl i t h i umb o r a t eg l a s sm a t r i x .J Ma t e rS c i L e t t 19 9 9 , 1 8:16 8 7– 1 69 0 . [3 ]B o r r e l l i NF ,L a y t on MM .E l e c t r o op t i cp r o p e r t i e so f t r a n s p a r e n tf e r r o e l e c t r i c g l a s s – c e r am i c s y s t em s . IEEETE l e c t r onD e v1 96 9 ,16 :5 1 1 – 51 4 . [4 ]B e l lA J .F e r ro e l e c t r i c s :Th ero l eo fc e r am i cs c i en c e and e ng i n e e r i ng .J E u r C e ram So c20 0 8 , 2 8: 13 0 7– 1 31 7 . [5 ]P engp a tK , Ho l l and D .F e r ro e l e c t r i cg l a s sc e r am i c s – N b O s y s t e m . J E u r C e r a m f r omth eP bO –G eO 2 2 5 So c2 0 04 , 24:29 5 1– 2 95 8 . [6 ]G r a ç a MPF ,d aS i lv a MGF ,V a l en t e MA .S t ru c t u r a l L i O–N b2O5 g l a s s a n de l e c t r i c a lp r o p e r t i e so fS iO 2– 2 and g l a s s c e r am i c s ob t a in ed by t h e rm o e l e c t r i c t r e a tm e n t s .J Ma t e rS c i2 0 0 7 , 4 2:2 5 43 – 25 50 . [7 ]G r a ç a MPF ,V a l e n t e MA ,d aS i l v a MGF .T h ee l e c t r i c b e h a v i o ro fal i t h i um –n i ob a t e –p ho s p h a t eg l a s sa n d g l a s s c e r am i c s .J M a t e rS c i2 0 06 , 41:1 1 37 – 1 14 1 . Jou rna lo fAd va n c edC e ram i c s2 014 ,3 (3 ) :194–2 06 [8 ]S h a nk a r MV , V a rm a KBR . C r y s t a l l i z a t i on o f O – V O – f e r ro e l e c t r i cb i sm u t hv an a d a t ei n B i 2 3 2 5 l a s s e s . JN o n -C r y s t So l i d s1 9 9 8 , 2 26: S rB4O7 g 14 5 –1 5 4 . [9 ]P en gp a tK ,H o l l a nd D .G l a s s c e r am i c scon t a i n i ng eO5) .J E u r f e r ro e l e c t r i cb i sm u t hg e rm an a t e(B i 2G C e r amS o c2 0 03 , 23:1 59 9 –1 60 7 . [1 0 ]R u i z -V a l d é sJ J ,G o r o kh o vs k y AV ,E s c a l a n t e -G a r c ı a ́ J I ,e ta l .G l a s s c e r am i c m a t e r i a l sw i thr egu l a t ed d i e l e c t r i cp r o p e r t i e sb a s e do nt h es y s t emB aO –P bO – –A l u rC e ram So c2 00 4 , 2 4: T iO2–B 2O3 2O3.J E 15 0 5– 1 50 8 . [1 1 ]B e ng i s uM ,B row RK , W i t t e n a u e rA .G l a s s e sa nd g l a s s c e r am i c sint h eS rO–T iO l S iO2–B 2–A 2O3– 2O3 d d i t i on s .J Ma t e rS c i sy s t emandth ee f f e c to fP 2O5 a 20 0 8 ,4 3:3 5 31 –3 5 38 . [1 2 ]Su bb a r a o EC . Af am i l yo ff e r ro e l e c t r i cb i sm u t h com pou nd s .JPh y sC h emSo l i d s19 6 2 , 2 3:6 65 – 67 6 . [1 3 ]D eA r a u jo CA , Cu c h i a r oJ , M cm i l l an LD ,e ta l . F a t igu e f r e ef e r ro e l e c t r i cc ap a c i t o r sw i t hp l a t i num e l e c t rod e s .N a t u r e1 99 4 ,3 7 4:62 7 –6 2 9 . [1 4 ]P a r k BH ,K a ng BS ,B u SD ,e ta l .L a n t h a num s ub s t i t u t e db i sm u t ht i t a n a t ef o ru s ei nn o n v o l a t i l e m em o r i e s .N a t u r e1 99 9 ,4 0 1:68 2 –6 8 4 . [1 5 ]T a k en a k aT ,N a g a t aH .C u r r e n ts t a t u sa n dp ro s p e c t s o fl e a d f r e ep i e z oe l e c t r i cc e r am i c s .JEu rC e ramSo c 20 0 5 ,2 5:2 6 93 –2 7 00 . [1 6 ]Ko j im aS ,H u s hu rA ,J i a n gF ,e ta l .C ry s t a l l i z a t i ono f am o rp h ou sb i sm u t ht i t a n a t e .JN o n -C r y s tS o l i d s2 0 01 , 29 3 –2 9 5:2 5 0– 25 4 . [1 7 ]Su n ah a r aK ,Y a n oJ ,K a k e g aw aK .P r ep a r a t i ono f i3O12 p a r t i c l e s by c r y s t a l l i z a t i onf r om g l a s s . B i4T JEu rC e ramSo c20 0 6 , 2 6:6 23 – 62 6 . i3O12f r om [1 8 ]G e r t hK ,R ü s s e lC .C r y s t a l l i z a t i ono fB i4T iO B JN on -C r y s t g l a s s e si nt h es y s t emB i2O3/T 2/ 2O3. So l i d s19 9 7 , 2 21:1 0– 1 7 . [1 9 ]B ru t o n TM .S t udy o ft h el i qu i d u si nt h esy s t em iO2.JSo l i dS t a t eC h em19 7 4 , 9:17 3 –1 7 5 . B i2O3–T iNbO9 [2 0 ]G e r t hK ,R ü s s e lC .C r y s t a l l i z a t i on o fB i3T T iO b B f romg l a s s e si nt h esy s t em B i 2O3/ 2/N 2O5/ 2O3/ o n -C r y s tS o l i d s19 9 9 , 2 4 3:5 2 –6 0 . S iO2.JN [2 1 ]K r a p c h a n s k aM ,D im i t r i e vY ,I o r d a no v aR . Ph a s e O – T i O – S i O . J o u r n a l fo rm a t ioni nt h esy s t em B i 2 3 2 2 o ft h e U n i v e r s i t yo f C h em i c a lT e c h n o l og ya n d M e t a l l u r g y 20 06 , 41:3 07 – 31 0 . [2 2 ]T a ng Q -Y , K a n Y -M , W a ng P -L ,e ta l . Nd /V i3O12 pow e rp r ep a r edby m o l t e ns a l t co d op e dB i 4T syn th e s i s .JAmC e r amS o c2 00 7 ,9 0:33 5 3– 33 5 6 . [2 3 ]Ko j im aT ,S a k a iT , W a t a n ab eT , e ta l .L a r g e T i O e p i t a x i a l r em a n en t po l a r i z a t i on o f(B i ,Nd ) 4 3 12 t h i nf i lm sg r ow n by m e t a l o r g a n i cc h em i c a lv a p o r d e p o s i t i o n .A p p lP h y sL e t t 20 02 , 80:2 74 6 . 205 [2 4 ]K imJK ,K im SS ,K im W J .E f f e c t so fann e a l in g c on d i t i on s o n t h e e l e c t r i c a l p r op e r t i e s o f i3O12 ( x=0 . 4 6 )t h i nf i lm sp ro c e s s e da tl ow B i4xNdxT t em p e r a tu r e .A pp lPh y sA 2 00 6 , 8 2:7 3 7– 7 40 . [2 5 ]S ak am o to W ,Y am a d aM ,I i z aw aN ,e ta l .P r ep a r a t i o n N d T i O t h i n f i l m s b y a nd p r o p e r t i e so f B i 4x x 3 12 c h em i c a ls o l u t i ond e p o s i t i o n .JE l e c t r o c e r am2 0 04 , 13:3 39 – 34 3 . [2 6 ]W uD ,L iA , M i n gN .S t r u c t u r ea nd e l e c t r i c a l i3O12f e r r o e l e c t r i cth in p r o p e r t i e so fo fB i3.15Nd0.85T f i lm s .JApp lP h y s2 00 4 ,9 5:4 27 5 . [2 7 ]M a iw a H , I i z aw a N , T og aw a D ,e t a l. i3O12 E l e c t r om e c h a n i c a lp r o pe r t i e so fN d d o p e dB i 4T f i lm s : A c a nd i d a t e f o r l e a d f r e e t h i n f i lm p i e zo e l e c t i c s .App lPh y sL e t t 20 0 3 , 8 2:1 7 60 –1 7 62 . [2 8 ]Suy a l G , B h a r adw a j a SSN , C a n ton i M ,e ta l . P r o p e r t i e s o f c h em i c a l s o l u t i on d e po s i t e d i3O12. po l y c r y s t a l l i n e n e ob i d i um -m od i f i e d B i 4T JE l e c t r o c e r am2 00 2 ,9:1 87 – 19 2 . [2 9 ]G a oXS ,X u eJM ,W a n gJ .F e r r o e l e c t r i cb e h a v i o ra n d i3O12t h i nf i lm s . ch a r g ec a r r i e r sin Nd -dop e dB i 4T JApp lP h y s2 0 05 , 97:0 34 1 01 . [3 0 ]Ch en M ,L iu ZL , W a ng Y ,e ta l .F e r ro e l e c t r i c do p e d p r o p e r t i e s an d m i c ro s t ru c t u r e so f N d2O3i3O12 c e r am i c s .P h y sS t a t u sS o l i d ia 2 0 03 ,2 0 0: B i4T 44 6 –4 5 0 . [3 1 ]V e rn a c o t a l aDE ,C h a t l an iS , Sh e l byJE .Ap p l i c a t i on s o ff e r ro e l e c t r i c s .P r o c e ed i n g so fth e 12 thIEEE I n t e r na t i o n a l S ym p o s i um on A p p l i c a t i on s o f F e r r o e l e c t r i c .H o n o l u l u ,H aw a i i ,USA ,20 00 . [3 2 ]Sh a nk a r MV ,V a rm a KBR .C ry s t a l l i z a t ion ,d i e l e c t r i c ando p t i c a ls tud i e sons t ro n t i umt e t r abo r a t eg l a s s e s c on t a i n i ngb i sm u t ht i t a n a t e .M a t e rR e sB u l l1 99 8 ,3 3: 17 6 9– 1 78 2 . [3 3 ]M o l l a AR ,T a r a f d e rA ,K a rm a k a rB .S y n t h e s i sa nd O – S i O – B i O – T i O2 p rop e r t i e so fg l a s s e si nt h eK 2 2 2 3 T i O ) n a n o s y s t em a nd b i sm u t ht i t a n a t e (B i 4 3 12 g l a s s– c e r am i c s th e r e o f .J M a t e rS c i2 0 1 1 ,4 6: 29 6 7– 2 97 6 . [3 4 ]G o l e z a r d iS ,M a r g hu s s i a n VK ,B e i t o l l a h iA ,e ta l . C ry s t a l l i z a t i on b eh a v i o r , m i c ro s t ru c t u r e a nd d i e l e c t r i cp r o p e r t i e so fl e a dt i t a n a t eg l a s sc e r am i c si n O a s a n u c l e a t i n g a g e n t . J E u r t h ep r e s e n c eo fB i 2 3 C e r amS o c2 0 10 ,30:1 45 3 –1 46 0 . [3 5 ]R e ddy AA ,T u l y a g a no v DU ,K a p o o rS ,e ta l .S t udy o f m e l i l i t e b a s e d g l a s s e s a n d g l a s sc e r am i c s O f o r f u n c t i o n a l a p p l i c a t i o n s . R S C nu c l e a t e dbyB i 2 3 Ad v2 01 2 ,2:1 09 5 5– 1 09 6 7 . [3 6 ]E l -M e l i e gy E ,v a nN o o r tR .G la s s e s and G la s s C e r am i c sf o r M e d i c a lA p p l i c a t i on s. N ew Y o r k : S p r i n g e r ,2 01 2 . [3 7 ]G au t am CR , Kum a r D ,P a r k a sh O . C on t r o l l ed 206 c r y s t a l l i z a t i on o f (P b ,S r )T iO o r o s i l i c a t eg l a s s 3b O . G l a s s P h y s C h e m + c e r am i c s dop e dw i t h Nb 2 5 20 1 3 ,3 9:1 6 2– 17 3 . [3 8 ]G au t am CR , Kum a rD ,P a r k a s hO .C ry s t a l l i z a t ion b eh a v i o ra nd m i c ro s t ru c t u r a lan a l y s i so fl e ad r i c h S r ) T i O g l a s s c e r a m i c s c o n t a i n i n g 1 m o l e% (Pb x 1x 3 v a n c e s i n M a t e r ia l s S c i e n c e and L a2O3. Ad En g i n e e r i n g2 0 1 1 , 20 1 1:4 0 2 37 6 . [3 9 ]G au t am CR , Kum a rD ,P a r k a s hO .C ry s t a l l i z a t ion b eh a v i o r a n d m i c ro s t ru c t u r a l an a l y s i s o f S r ) T i O g l a s s c e r a m i c s i n s t ro n t ium r i ch (Pb x 1x 3 O . A d v a n c e s i n M a t e r i a l s S c i e n c e p r e s e n c eo fL a 2 3 an dEn g i n e e r i ng2 0 1 1 ,2 01 1:7 47 3 46 . [4 0 ]G au t am CR , Y a d av AK , S i n g h P . Sy n t h e s i s , c ry s t a l l i z a t i on an d m i c ro s t r u c t u r a l s t udy o f o r o s i l i c a t eg l a s sc e r am i c p e r o v sk i t e(B a ,S r )T iO 3b a t e rR e sInno v 20 1 3 ,1 7: do p e d w i t hL a2O3.M 14 8 –1 5 3 . [4 1 ]P a t t e r so n AL . Th eS c h e r r e rf o rm u l a fo r X r ay Jou rna lo fAd va n c edC e ram i c s2 014 ,3 (3 ) :194–2 06 p a r t i c l es i z ed e t e rm i n a t i on . Ph y sR e v1 93 9 , 56: 97 8 –9 8 2 . [4 2 ]S a h u AK ,K um a rD ,P a r k a s hO .C r y s t a l l i z a t i ono f l e a d s t r on t i um t i t a n a t e p e r o v sk i t e p h a s e i n S rx)O ·T iO – [ 2S iO ·B O3] – [K ] g l a s s [ (P b 1x 2] 2 2 2O c e r am i c s .Ad vApp lC e ram 2 0 03 , 10 2:13 9 –1 47 . [4 3 ]B a h r am i a A , N em a t i ZA , A l i z a d e h P , e ta l . C ry s t a l l i z a t ion and e l e c t r i c a l p rop e r t i e s o f S rx) ·T iO [ (2S iO ·B ) ] [K O ]g l a s s – c e r am i c s . [ (P b 1x 3] 2 2O3 2 J Ma t e rP r o c e s sT e c h2 00 8 ,2 06:1 26 – 13 1 . [4 4 ]Kum a rD ,G a u t am CR ,P a rk a s hO .P r e p a r a t ionan d d i e l e c t r i c c h a r a c t e r i z a t i o n o f f e r r o e l e c t r i c S r1x)T iO l a s sc e r am i c s dop ed w i th L a2O3. (Pb x 3g App lPh y sL e t t 20 0 6 , 8 9:1 1 2 9 08 . [4 5 ]G au t am CR ,S i ng hP ,T h a k u r OP ,e ta l .Sy n t h e s i s , s t ru c tu r eandim p ed an c es p e c t ro s c op i ca n a ly s i so f S r1x) ·OT iO – [ (2S iO ·B ] – 7 [B aO ] – 3 [K ] [ (P b x 2] 2 2O3) 2O .J Ma t e rS c i g l a s sc e r am i csy s t emdop e dw i t hL a 2O3 20 1 2 ,4 7:6 6 52 –6 6 64 .