Effects of Bi Excess on the Preferred Orientation and Electrical Properties of (Bi 3.84 Nd 0.16 )Ti 3 O 12 Ceramics

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Effects of Bi Excess on the Preferred Orientation and Electrical Properties of (Bi _3.84 Nd _0.16 )Ti ₃ O ₁₂ Ceramics

Do Hyun Jeon · Sam Yeon Cho · Byung Hoon Kim · Sin Wook Kang · Jin Ho Kwak · Sun A Yang · Sang Don Bu ^∗

Department of Physics and Research Institute of Physics and Chemistry, Chonbuk National University, Jeonju 561-756, Korea

Gyoung Ja Lee · Min Ku Lee ^†

Nuclear Materials Development Division, Korea Atomic Energy Research Institute, Daejeon 305-535, Korea (Received 16 June 2014 : revised 20 June 2014 : accepted 21 June 2014)

(Bi

3.84

Nd

0.16

)Ti

3

O

12

(BNdT) ceramics with different excess bismuth (Bi) contents from 0 mol%

to 20 mol% were prepared by using the solid-state reaction method. No secondary phases were in any of the ceramics. The amount of a-axis orientation changed with increasing excess Bi contents, and the maximum a-axis orientation was observed in the BNdT ceramic with 5 mol% excess Bi content. The value of the remanent polarization of the ceramics also changed with changing excess of Bi content, and the maximum value of the remanent polarization was observed in the ceramic with 5 mol% excess Bi content. The change in the behavior of the remanent polarization was observed to be similar to that of the a-axis orientation, which suggests that the amount of a- axis orientation highly affects ferroelectric properties such as the remanent polarization in BNdT ceramics. The maximum phase-transition temperature (T

c

) was observed to be 632

^◦

C in the BNdT ceramic without excess Bi content, and the T

c

was observed to decrease continuously to 616

^◦

C with increasing excess Bi content. From these results, we can conclude that a 5 mol% excess Bi content to enhances the electrical properties of BNdT ceramics favor.

PACS numbers: 77.84.Cg, 77.80.-e, 77.22.-d, 68.55.jm, 68.55.Ln

Keywords: Ferroelectrics, BIT, Ceramics, Dielectric property, Preferred orientation

Bi Y 8 ÈS ë s; c Â \ ¥ (Bi 3.84 Nd _0.16 )Ti ₃ O ₁₂ : g Ã k Ä 8 ý 9 0] §V R Ë õ m Í ¹ ÅM X ì Ä ¤V R Ë ì Å× D

b 9

| ¡g ` @ · Ð a : @ · »( å 0 å · ~ ç ¡ , > ] 8 ; · + 2 . > Ú · è ¡` 9 · « » ç ¡% ã < ^∗

· ¡ ¤ @ / < Æ § Ó ü t o < Æõ , Å Ò 561-756

T

# Ü · T * > ¦ ^†

ô

Ç² D G" é ¶ § 4 ½ ¨" é ¶ " é ¶ § 4 F « Ñ> hµ 1 ÏÂ Ò, @ / 305-535

(2014¸ 6 Z 4 16{ 9 ~ Ã Î6 £ §, 2014¸ 6 Z 4 20{ 9 Ã º& ñ : r ~ Ã Î6 £ §, 2014¸ 6 Z 4 21{ 9 > F S X & ñ )

Bi\ ¦ 0 mol% \ " f 20 mol% t # 3 0 A\ " f õ e ç ' ô Ç (Bi

3.84

+Nd

0.16

)Ti

3

O

12

(BNdT) [ j b ` ¦

¦ © ì ø Í6 £ xZ O Ü ¼ Ð ] j % i . ¸ H r « Ñ\ " f s © _ + þ A$ í É r ' a ¹ 1 Ï ÷ &t · ú § ¤ . Bi ' | ¾ Ós 7 £ x < Ê

\

" f a-» ¡ ¤ ~ ½ Ó ¾ Ó _ C ¾ Ó$ í s o H כ ` ¦ S X % i Ü ¼ 9, a-» ¡ ¤ ~ ½ Ó ¾ Ó _ C ¾ Ó$ í _ þ j@ / ° ú כ É r 595

This is an Open Access article distributed under the terms of the Creative Commons Attribution Non-Commercial License

(http://creativecommons.org/licenses/by-nc/3.0) which permits unrestricted non-commercial use, distribution, and reproduction in any

medium, provided the original work is properly cited.

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¹ Ï % Ü ¼ 9, s ~ Ó Ó _ C Ó$ í s BNdT [ j b _ ï À Óì õ ° ú y Ä »

$ í

o\ H % ò ¾ Ó` ¦ p 2 ; H כ ` ¦ r ô Ç . © s : r ¸_ þ j@ /° ú כ É r 632

^◦

C Ð Bi õ e ç ' ÷ &

t

· ú § É r BNdT r « Ñ\ " f ' a ¹ 1 Ï ÷ &% 3 Ü ¼ 9, © s : r ¸ H Bi ' | ¾ Ós 7 £ x < Ê\ " f 616

^◦

C t t 5

Å q& h Ü ¼ Ð ± ú & . s Qô Ç õ [ þ t ÐÂ Ò' 5 mol%_ Bi õ e ç ' BNdT [ j b r « Ñ_ l & h :

£ ¤$ í ¾ Ó © \ © Ä »o > 6 x H כ Ü ¼ Ð ó ø Íé ß ) a .

PACS numbers: 77.84.Cg, 77.80.-e, 77.22.-d, 68.55.jm, 68.55.Ln Keywords: [ j b Û ¼, q Û ¼Á ºÛ ¼ 8 £ x © ½ ¨ ¸, q Û ¼Á ºÛ ¼ õ e ç '

I. " e Â ] Ø

y

© Ä » ^ [ j b É r Z } É r Ä » : £ ¤$ í õ · ú : £ ¤$ í , Õ ª o

¦ y © Ä » : £ ¤$ í ` ¦ ° ú l M :ë H \ » ¡ ¤ l , q 6 fµ 1 Ï$ í B j ¸ o

Õ ªo ¦ G ' p" f 1 p x \ 6 £ x6 x| ¨ c Ã º e . : £ ¤ y , @ /³ ð& h y © Ä

» ^ Ó ü t| 9 Pb(Zr,Ti)O 3 (PZT)\ ¦ s 6 x ô Ç [ j b É r Ä

ºÃ ºô Ç y © Ä » $ í õ · ú $ í ` ¦ ? /# Q © \ O & h Ü ¼ Ð # Q ì

r \ s 6 x ÷ & ¦ e . Õ ª Q PZT_ â Ä º © s : r ¸ (T c ) 350 ^◦ C & ñ ¸ Ð, z ´F & h Ü ¼ Ð 150 ^◦ C s _ z ´ : r

¨ 8

â \ " fë ß è Ð s 6 x 0 p x . " f, þ j H ¦ : r ¨ 8

â

\ " f 1 l x H [ j b è \ ¦ > µ 1 Ï l 0 Aô Ç ½ ¨[ þ t s

' ÷ & ¦ e [1]. ¦ : r ¨ 8 â \ " f 6 x l 0 AK " f H Ó ü t

| 9

_ © s : r ¸ Z } H X <, y © Ä » ^ Ó ü t| 9 × æ q Û

¼Á ºÛ ¼ 8 £ x © ½ ¨ ¸\ ¦ t H Bi 4 Ti ₃ O ₁₂ (BIT) Ó ü t| 9 É r

É

r y © Ä » ^ Ó ü t| 9 \ q K © @ /& h Ü ¼ Ð Z } É r © s : r ¸

\

¦ t ¦ e .

q

Û ¼Á ºÛ ¼ 8 £ x © ½ ¨ ¸ y © Ä » ^ BIT H (Bi 2 O 2 ) ²⁺ (A m−1 B m O 3m+1 ) ²⁻ Ü ¼ Ð ³ ð & ³÷ & 9, A o

ü < B o \ y y Biü < Ti 0 Au K e ¦, q Û ¼Á ºÛ ¼ 8

£

x s \ 3> h_ ` ÐÚ ÔÛ ¼ s à Ô 8 £ x s Á ú ¢# e H ½ ¨ ¸

\

¦ s À Ò ¦ e . BIT [ j b É r PZT [ j b , KNN [ j b

Ð ± ú É r · ú , y © Ä » : £ ¤$ í ` ¦ Ðs l M :ë H \ La, Nd, Sm ° ú É r B ÐÀ Ó\ ¦ ' K " f : £ ¤$ í ` ¦ > h 9 H

½

¨ ´ ú §s ' ÷ & ¦ e [2]. Õ ª × æ \ " f Nd\ ¦ '

y © Ä » : £ ¤$ í õ Ä » : £ ¤$ í s a % ~ t H õ µ 1 Ï³ ð÷ &

%

3 [3]. Õ ª Q BIT> [ j b ` ¦ ] j l 0 AK " f H Z

} É r : r ¸\ " f è ` ¦ K ¦, s õ & ñ \ " f Ô ¦ î ß & ñ ô Ç Bi ~ 1 > 6 fµ 1 Ï÷ & H ë H ] j e [4]. Bi_ 6 fµ 1 Ï Ð K

ª s : r < Ês Ò q t$ í ÷ & ¦, s Qô Ç < Ê É r ì r F

G x Ð & ³ © ¢ ¸ H ¾ º[ O À Ó 1 p x` ¦ 7 £ x r & Ó ü t| 9 _ y © Ä

» : £ ¤$ í x 9 l & h : £ ¤$ í \ É r % ò ¾ Ó` ¦ p 2 ; .

∗

E-mail: [email protected]

†

E-mail: [email protected]

"

f Bi\ ¦ õ e ç ' # Bi_ 6 fµ 1 Ï` ¦ Ð © #

< Ê` ¦ y èr & : £ ¤$ í ` ¦ > h r v H ½ ¨[ þ t s Ö ¸ µ 1 Ï >

' ÷ & ¦ e [5]. : r ½ ¨\ " f H l & h : £ ¤$ í s Ä ºÃ º ô

Ç ¸$ í ` ¦ % 3 l 0 AK BIT\ Nd\ ¦ ' ô Ç BNdT [ j b

\ Bi\ ¦ õ e ç ' # ¦ © ì ø Í6 £ xZ O Ü ¼ Ð ] j % i .

]

j ) a BNdT [ j b \ " f q Û ¼Á ºÛ ¼ 8 £ x © ` ÐÚ ÔÛ ¼ s à

Ô © + þ A$ í É r X- r] X (X-ray diffraction, XRD)` ¦ : x K

S X % i . Õ ªo ¦ Ä » © Ã º, Ä » < Hz ´, ï ß À Óì rF G Õ

ªo ¦ ½ Ó l © ` ¦ 8 £ ¤& ñ # Bi _ õ e ç ' | ¾ Ó\ É r T _c ü < l & h : £ ¤$ í x 9 y © Ä » : £ ¤$ í ` ¦ ¸ % i .

II. ÷ m Ç ] M ö

Bi 2 O 3 (99.9%, Sigma Aldrich), Nd 2 O 3 (99.9% Sigma Aldrich), TiO ₂ (99.9% Sigma Aldrich) ì r ´ ú ` ¦ " é ¶ « Ñ Ð ¦

© ì ø Í6 £ xZ O Ü ¼ Ð Bi\ ¦ õ e ç ' ô Ç BNdT [ j b ` ¦ ] j ¸

%

i . BNdT [ j b É r Bi 3.84 Nd 0.16 Ti 3 O 12 ¸$ í q Ð Bi\ ¦ 0 mol% \ " f 20 mol% t õ e ç ' % i . Bi õ e ç '

| ¾ Ó\ BNdT [ j b ` ¦ y y BNdT-0%, BNdT-5%, BNdT-10%, BNdT-15% Õ ªo ¦ BNdT-20%Ü ¼ Ð " î % i

. " é ¶ « Ñì r ´ ú õ \ ò ø Í` ¦ õ t Ø Ô ïm ^ ¦` ¦ [ O # Q 12r ç ß 1

l

x î ß 1 ^ ¦x 9 Ð D ¥ ½ + Ë % i ¦, 120 ^◦ C \ " f Ø æì r y | ¸

% i . | ¸ ) a ì r ´ ú ` ¦ · ú À Òp ¸m \ V , ¦ 740 ^◦ C

\

" f 2r ç ß 1 l x î ß 1 è % i . è ) a ì r ´ ú ` ¦ 0 A õ

&

ñ õ 1 l x{ 9 ô Ç ¸| Ü ¼ Ð 2 ^ ¦x 9 ` ¦ ¦ | ¸ô Ç Ê ê 2

è % i . 2 è = å Q è ß ì r ´ ú \ 5 wt% polyviny- lalcohol (PVA)\ ¦ D ¥ ½ + Ë # Ä »µ 1 Ï Ð ì r W # ^ è H ß ¼l

100 µm ^ Ð ^ 2 £ § % i . Õ ª + '\ 10 mm F K + þ

Ad ¦ \ " f · ú $ í + þ Aô Ç Ê ê 1100 ^◦ C \ " f 2r ç ß 1 l x î ß è

% i . è Ê ê r « Ñ[ þ t _ l & h : £ ¤$ í ` ¦ 8 £ ¤& ñ l 0

AK 500 µm Ð / B N ¦ É r (Ag) F G` ¦ 7 £ x Ã Ì % i .

X- r] X © u (XRD, RIGAKU MAX-2500)\ ¦ s 6 x K

"

f Bi 3.84 Nd 0.16 Ti 3 O 12 [ j b _ & ñ ½ ¨ ¸\ ¦ ì r$ 3 % i

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Fig. 1. (Color online) XRD patterns of BNdT ceramics with different excess bismuth concentrations sintered at 1100 ^◦ C.

. Piezoelectric evaluation system (PES, aixACT aix- PES)` ¦ s 6 x # ô Ç l © \ É r y © Ä » s § 4 / B G

` ¦ 8 £ ¤& ñ % i ¦, e x ~ Û ¼ ì r$ 3 l (HP4194A)\ ¦ s 6 x

# 100 Hz - 10 MHz Å Ò Ã º # 3 0 A\ " f © : r Â Ò' 700

◦ C t Ä » © Ã ºü < Ä » < Hz ´` ¦ 8 £ ¤& ñ % i .

III. ÷ m Ç] M ö+ s ÇÊ Ý õ m Í w ² o

Figure 1 É r Bi ' | ¾ Ó\ É r BNdT-0%, BNdT-5%, BNdT-10%, BNdT-15% Õ ªo ¦ BNdT-20% [ j b _ X-

r] X Á º] (\ ¦ 2θ = 10 ∼ 70 ^◦ _ r] X y # 3 0 A\ " f 8 £ ¤& ñ ô Ç

õ s . ¸ H r « Ñ\ " f Bi õ e ç ' \ É r s © É r S X

÷ &t · ú § ¤Ü ¼ 9, ~ ½ Ó& ñ > ½ ¨ ¸_ Bi ^3.6 Nd 0.4 Ti 3 O 12

(JCPDS No. 36-1486) ü < 1 l x{ 9 ô Ç ½ ¨ ¸\ ¦ ? /% 3 . Bi '

| ¾ Ós 7 £ x < Ê\ " f BNdT-0%\ " f BNdT-15% t

_ r « Ñ\ " f H XRD © \ " f H o t · ú § ¤ t

ë ß , BNdT-20% r « Ñ H É r r « Ñ\ q K (006), (008), (0014) Õ ªo ¦ (0016) ~ ½ Ó ¾ Ó _ x ß ¼ (peak) [ jl © @ /

&

h Ü ¼ Ð ß ¼> 7 £ x % i . 0 A_ ~ ½ Ó ¾ Ó [ þ t É r / B N: x& h Ü ¼ Ð c-» ¡ ¤ Ü ¼ Ð $ í © ) a ½ ¨ ¸ Ð, s Qô Ç c-» ¡ ¤ ~ ½ Ó ¾ Ó [ þ t _ $ í © É r BNdT ~ Ã Ì} ` ¦ s 6 x ô Ç ' ½ ¨\ " f y © Ä » $ í \ % ò ¾ Ó` ¦ Å

Ò H כ Ü ¼ Ð Ð ¦ ÷ &% 3 [6]. s ü < ' aº # BNdT r

«

Ñ_ C ¾ Ó$ í ` ¦ S X l 0 A # , a-» ¡ ¤ Õ ªo ¦ c-» ¡ ¤ $ í ©

)

a ~ ½ Ó ¾ Ó [ þ t _ q Ö ¦` ¦ S X % i . a-» ¡ ¤ ~ ½ Ó ¾ Ó [ þ t _ q Ö

¦ (α (l00) ) É r 6 £ § _ d Ü ¼ Ð & ñ _ % i .

α (l00) = ΣI (n00) /ΣI (hkl) (1)

Fig. 2. (Color online) (a) Hysteresis loops of BNdT ce- ramics with different excess bismuth concentrations. (b) Variations of α _(l00) and 2P _r values of BNdT ceramics for different excess bismuth concentrations.

Õ

ªo ¦ c-» ¡ ¤ ~ ½ Ó ¾ Ó [ þ t _ q Ö ¦ (α (00l) ) _ d É r 6 £ § õ ° ú

.

α _(00l) = ΣI _(00n) /ΣI _(hkl) (2)

#

l " f, I (hkl) É r [ j b r « Ñ\ " f 8 £ ¤& ñ ) a (hkl) x ß ¼ [ jl s

¦, n É r ~ ½ Ó ¾ Ó _ Õ ü w \ ¦ _ p ô Ç . Bi ' | ¾ Ó\

"

f BNdT-0%, BNdT-5%, BNdT-10%, BNdT-15% Õ ªo

¦ BNdT-20% r « Ñ_ α (l00) H y y 5.1, 14.3, 10.0, 10.3 Õ

ªo ¦ 4.3% s % 3 Ü ¼ 9, α (00l) H 18.4, 17.1, 12.1, 16.1 Õ ª o

¦ 64.8% Ð S X ÷ &% 3 .

Figure 2 H Bi Ã Ð| ¾ Ó\ É r BNdT [ j b r « Ñ_ P − E s § 4 / B G ` ¦ · p כ s . Bi ' | ¾ Ó\ " f BNdT-0%, BNdT-5%, BNdT-10%, BNdT-15% Õ ªo ¦ BNdT-20% r « Ñ\ " f_ ï ß À Ó ì rF G (2P r , 2P _r = | P _r ⁺ + P _r ⁻ |) ° ú כ É r y y 10, 14, 11, 10 Õ ªo ¦ 3 µC/cm ² ° ú כ` ¦

Ð% i Ü ¼ 9, ½ Ó l © (2E c , 2E _c = | E _c ⁺ + E _c ⁻ |) ° ú כ É r y y

95, 84, 88, 93 Õ ªo ¦ 99 kV/cm ° ú כ` ¦ ? /% 3 . { 9 ì

ø Í& h Ü ¼ Ð P − E s § 4 / B G ` ¦ s 6 x ô Ç y © Ä » $ í _ ¨ î H Z

} É r ï ß À Ó ì rF G ° ú כõ ± ú É r ½ Ó l © ° ú כ` ¦ l ï r Ü ¼ Ð s À Ò

#

Q | 9 Ã º e . s Qô Ç ' a& h \ " f ¶ ú ( R Ð , Bi ' | ¾ Ós

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Fig. 3. (Color online) Frequency dependences of (a) di- electric constant, and (b) dielectric loss of BNdT ceram- ics with different excess bismuth concentrations.

7 £

x < Ê\ " f BNdT-0%\ ¦ l ï r Ü ¼ Ð BNdT-5% \

"

f © a % ~ É r y © Ä » $ í ` ¦ ? /% 3 BNdT-10% s

© \ " f H y © Ä » $ í s t 5 Å q& h Ü ¼ Ð y è % i . s Qô Ç y

© Ä » $ í _ o â ¾ Ó É r α (l00) _ o 1 l x õ Ä » ô Ç

õ \ ¦ Ð% i Ü ¼ 9, s \ É r P r ° ú כõ α (l00) _ o õ H Fig. 2(b) \ ? /% 3 . s \ ¦ : x K " f, c-» ¡ ¤ ~ ½ Ó ¾ Ó [

þ

t \ q K a-» ¡ ¤ ~ ½ Ó ¾ Ó [ þ t _ C ¾ Ó$ í s y © Ä » : £ ¤$ í \ ©

@

/& h Ü ¼ Ð ' a$ í s H כ Ü ¼ Ð Ò q ty ½ + É Ã º e Ü ¼ 9 [7, 8], Õ

ª Qô Ç " é ¶ É r BNdT\ ¦ í < Êô Ç Bi 8 £ x © ½ ¨ ¸ y © Ä » ^

° ú

H Z } É r q 1 p x ~ ½ Ó$ í \ l ô Ç . : £ ¤ y , c-» ¡ ¤ ~ ½ Ó ¾ Ó Ü ¼ Ð Z

} É r C ¾ Ó$ í ` ¦ Ðs H BNdT-20% r « Ñ_ â Ä º\ ©

± ú

Òכ ¹ > 6 x < Ê` ¦ S X ½ + É Ã º e H õ s . s ü @\

É r Bi ' | ¾ Ó\ É r ½ ¨ ¸& h o\ ¦ ¦ 9 ½ + É Ã º e .

7 £ ¤, BNdT-0% _ â Ä º, \ P % o õ & ñ \ " f Bi_ 6 fµ 1 Ï\ _ ô

, BNdT-5% \ " f õ e ç ' ) a Bi < Ê` ¦ G 0 >Å Ò# Q

Fig. 4. (Color online) Temperature dependences of di- electric constant of BNdT ceramics with different excess bismuth concentrations.

s

> ) a [9,10].

\

0.0109, 0.0035, 0.0032, 0.0030 Õ ªo ¦ 0.0094\ ¦

?

\

t 5 Å q& h Ü ¼ Ð y è % i . s Qô Ç õ [ þ t É r BNdT [ j

Ç þ j& h _ Bi ' | ¾ Ó É r 5 mol% H % e ` ¦ r ô Ç .

|

\

" f / B N: x& h Ü ¼ Ð H 630 ^◦ C Â Ò H _ Ä » Ö ¦ x ß ¼

~

õ [ þ t É r õ e ç ' ) a Bi s : r[ þ t s BNdT [ j b _

½

¨ ¸& h o\ x 9 ] X > ' a ÷ &# Q e 6 £ §` ¦ r ô Ç . Õ ª

¤ .

(5)

IV. + s Ç Â ] Ø

Bi y y 0, 5, 10, 15, 20 mol% Ð õ e ç ' ) a BNdT [

j b ` ¦ ] j # Bi ' | ¾ Ó\ É r p [ j½ ¨ ¸ oü <

l & h : £ ¤$ í ` ¦ S X % i . Bi ' | ¾ Ós 7 £ x < Ê\

ß À Óì rF G ° ú כ (14 µC/cm ² )` ¦ Ð% i . ì ø Í \ BNdT-10%

s

è H â ¾ Ó` ¦ ? /% 3 . ¢ ¸ô Ç, : r ¸\ _ > r H Ä »

s : r ¸ 632 ^◦ C \ " f 616 ^◦ C t ± ú t H כ ` ¦ S X

% i . s Qô Ç o_ " é ¶ É r BNdT [ j b _ C ¾ Ó

$ í

¾ Ó\ _ ô Ç כ Ü ¼ Ð # . " f, BNdT [ j b \ " f

P

c p 8 ý ò k >

This work was supported by the Nuclear Power Core Technology Development Program of the Korea Insti- tute of Energy Technology Evaluation and Planning (KETEP) granted financial resource from the Ministry of Trade, Industry & Energy, Republic of Korea (No.

20131520000210).

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Effects of Bi Excess on the Preferred Orientation and Electrical Properties of (Bi 3.84 Nd 0.16 )Ti 3 O 12 Ceramics

Effects of Bi Excess on the Preferred Orientation and Electrical Properties of (Bi 3.84 Nd 0.16 )Ti 3 O 12 Ceramics

Do Hyun Jeon · Sam Yeon Cho · Byung Hoon Kim · Sin Wook Kang · Jin Ho Kwak · Sun A Yang · Sang Don Bu ∗

Department of Physics and Research Institute of Physics and Chemistry, Chonbuk National University, Jeonju 561-756, Korea

Gyoung Ja Lee · Min Ku Lee †

Nuclear Materials Development Division, Korea Atomic Energy Research Institute, Daejeon 305-535, Korea (Received 16 June 2014 : revised 20 June 2014 : accepted 21 June 2014)

(Bi

Nd

)Ti

O

(BNdT) ceramics with different excess bismuth (Bi) contents from 0 mol%

) was observed to be 632

C in the BNdT ceramic without excess Bi content, and the T

was observed to decrease continuously to 616

C with increasing excess Bi content. From these results, we can conclude that a 5 mol% excess Bi content to enhances the electrical properties of BNdT ceramics favor.

PACS numbers: 77.84.Cg, 77.80.-e, 77.22.-d, 68.55.jm, 68.55.Ln

Keywords: Ferroelectrics, BIT, Ceramics, Dielectric property, Preferred orientation

Bi Y 8 ÈS ë s; c  Â \ ¥ (Bi 3.84 Nd 0.16 )Ti 3 O 12 : g Ã k Ä­ 8 ý 9 0]  §V R Ë õ m Í  ¹ ÅM X ì Ä  ¤V R Ë ì Å× D

b 9

| ¡g ` @ ·  Ð  a : @ ·  »( å 0 å  · ~ ç ¡ , > ] 8 ; ·  + 2 . >  Ú · è ¡` 9   · « » ç ¡% ã < ∗



 · ¡ ¤ @ / < Æ § Ó ü t o  < Æõ ,   Å Ò 561-756

T

# Ü   · T  * > ¦  †

ô

 Ç² D G" é ¶  § 4   ½ ¨" é ¶ " é ¶  § 4 F « Ñ> hµ 1 ÏÂ Ò, @ /  305-535

(2014¸  6 Z 4 16{ 9  ~ Ã Î6 £ §, 2014¸  6 Z 4 20{ 9  Ã º& ñ  : r ~ Ã Î6 £ §, 2014¸  6 Z 4 21{ 9  > F  S X & ñ )

Bi\  ¦ 0 mol% \ " f 20 mol% t  # 3 0 A\ " f õ e ç '  ô  Ç (Bi

+Nd

)Ti

O

(BNdT) [ j b  `  ¦



¦ © ì ø Í6 £ xZ O Ü ¼ Ð ] j   % i  .  ¸  H r « Ñ\ " f s   © _  + þ A$ í  É r  ' a ¹ 1 Ï ÷ &t  · ú §  ¤ . Bi '  | ¾ Ós  7 £ x  < Ê

\

   " f a-» ¡ ¤ ~ ½ Ó ¾ Ó  _  C  ¾ Ó$ í s    o   H  כ `  ¦ S X    % i Ü ¼ 9, a-» ¡ ¤ ~ ½ Ó ¾ Ó  _  C  ¾ Ó$ í _  þ j@ / ° ú כ É r 595

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 ¹ Ï % Ü ¼ 9, s  ~ Ó Ó _  C  Ó$ í s  BNdT [ j b  _  ï À Óì õ  ° ú  y Ä »

$ í

  o\   H % ò  ¾ Ó`  ¦ p  2 ;   H  כ `  ¦ r  ô  Ç .  ©   s   : r  ¸_  þ j@ /° ú כ É r 632

C  Ð Bi õ e ç '  ÷ &

t

 · ú § É r BNdT r « Ñ\ " f  ' a ¹ 1 Ï ÷ &% 3 Ü ¼ 9,  ©   s   : r  ¸  H Bi '  | ¾ Ós  7 £ x  < Ê\    " f 616

C  t  t  5

Å q& h Ü ¼ Ð ± ú   &   . s  Qô  Ç   õ [ þ t  ÐÂ Ò'  5 mol%_  Bi õ e ç '   BNdT [ j b  r « Ñ_    l & h :

£ ¤$ í  ¾ Ó © \   ©  Ä »o  >    6 x   H  כ Ü ¼ Ð ó ø Íé ß   ) a .

PACS numbers: 77.84.Cg, 77.80.-e, 77.22.-d, 68.55.jm, 68.55.Ln Keywords: [ j b  Û ¼, q Û ¼Á ºÛ ¼ 8 £ x  © ½ ¨ ¸, q Û ¼Á ºÛ ¼ õ e ç '  

I. " e Â ] Ø

y

© Ä »  ^  [ j b   É r Z  } É r Ä »  : £ ¤$ í õ  · ú   : £ ¤$ í , Õ ª o

 ¦ y © Ä »  : £ ¤$ í `  ¦ ° ú l  M :ë  H \  » ¡ ¤  l , q 6 fµ 1 Ï$ í B j ¸ o

 Õ ªo  ¦ G ' p" f 1 p x \  6 £ x6 x| ¨ c Ã º e   . : £ ¤ y , @ /³ ð& h   y ©  Ä

»  ^  Ó ü t| 9   Pb(Zr,Ti)O 3 (PZT)\  ¦ s 6 x ô  Ç [ j b   É r Ä

ºÃ ºô  Ç y © Ä »  $ í õ  · ú   $ í `  ¦  ? /# Q  © \ O & h Ü ¼ Ð #  Q ì

 r  \  s 6 x ÷ & ¦ e   . Õ ª Q  PZT_   â Ä º  ©   s   : r  ¸ (T c )  350 ◦ C & ñ  ¸ Ð, z ´F & h Ü ¼ Ð 150 ◦ C s  _  z ´ : r

¨ 8

 â \ " fë ß   è  Ð s 6 x 0 p x  .   " f, þ j   H  ¦ : r ¨ 8 

 â

\ " f   1 l x   H [ j b   è \  ¦ > µ 1 Ï l  0 Aô  Ç   ½ ¨[ þ t s 



 '  ÷ & ¦ e    [1].  ¦ : r ¨ 8  â \ " f  6 x l  0 AK " f  H Ó ü t

| 9

_   ©   s   : r  ¸ Z  }      H X <, y © Ä »  ^  Ó ü t| 9  ×  æ q  Û

¼Á ºÛ ¼ 8 £ x  © ½ ¨ ¸\  ¦ t   H Bi 4 Ti 3 O 12 (BIT) Ó ü t| 9  É r 

 É

r y © Ä »  ^  Ó ü t| 9 \  q K   © @ /& h Ü ¼ Ð Z  } É r  ©   s   : r  ¸

\

 ¦ t  ¦ e   .

q

Û ¼Á ºÛ ¼ 8 £ x  © ½ ¨ ¸ y © Ä »  ^   BIT  H (Bi 2 O 2 ) 2+ (A m−1 B m O 3m+1 ) 2− Ü ¼ Ð ³ ð & ³÷ & 9, A   o

ü < B o \  y  y   Biü < Ti  0 Au K  e   ¦, q Û ¼Á ºÛ ¼ 8

£

x  s \  3> h_  `  ÐÚ ÔÛ ¼ s à Ô 8 £ x s  Á ú ¢#  e    H ½ ¨ ¸

\

 ¦ s À Ò ¦ e   . BIT [ j b   É r PZT [ j b  , KNN [ j  b 

 Ð  ± ú  É r · ú   , y © Ä »  : £ ¤$ í `  ¦  Ðs l  M :ë  H \  La, Nd, Sm ° ú  É r B ÐÀ Ó\  ¦ '  K " f : £ ¤$ í `  ¦ > h   9  H  

½

¨ ´ ú §s    '  ÷ & ¦ e    [2]. Õ ª ×  æ \ " f Nd\  ¦ '   

Effects of Bi Excess on the Preferred Orientation and Electrical Properties of (Bi _3.84 Nd _0.16 )Ti ₃ O ₁₂ Ceramics

Do Hyun Jeon · Sam Yeon Cho · Byung Hoon Kim · Sin Wook Kang · Jin Ho Kwak · Sun A Yang · Sang Don Bu ^∗

Gyoung Ja Lee · Min Ku Lee ^†

Bi Y 8 ÈS ë s; c Â \ ¥ (Bi 3.84 Nd _0.16 )Ti ₃ O ₁₂ : g Ã k Ä 8 ý 9 0] §V R Ë õ m Í ¹ ÅM X ì Ä ¤V R Ë ì Å× D

| ¡g ` @ · Ð a : @ · »( å 0 å · ~ ç ¡ , > ] 8 ; · + 2 . > Ú · è ¡` 9 · « » ç ¡% ã < ^∗

· ¡ ¤ @ / < Æ § Ó ü t o < Æõ , Å Ò 561-756

# Ü · T * > ¦ ^†

Ç² D G" é ¶ § 4 ½ ¨" é ¶ " é ¶ § 4 F « Ñ> hµ 1 ÏÂ Ò, @ / 305-535

(2014¸ 6 Z 4 16{ 9 ~ Ã Î6 £ §, 2014¸ 6 Z 4 20{ 9 Ã º& ñ : r ~ Ã Î6 £ §, 2014¸ 6 Z 4 21{ 9 > F S X & ñ )

Bi\ ¦ 0 mol% \ " f 20 mol% t # 3 0 A\ " f õ e ç ' ô Ç (Bi

(BNdT) [ j b ` ¦

¦ © ì ø Í6 £ xZ O Ü ¼ Ð ] j % i . ¸ H r « Ñ\ " f s © _ + þ A$ í É r ' a ¹ 1 Ï ÷ &t · ú § ¤ . Bi ' | ¾ Ós 7 £ x < Ê

" f a-» ¡ ¤ ~ ½ Ó ¾ Ó _ C ¾ Ó$ í s o H כ ` ¦ S X % i Ü ¼ 9, a-» ¡ ¤ ~ ½ Ó ¾ Ó _ C ¾ Ó$ í _ þ j@ / ° ú כ É r 595

¹ Ï % Ü ¼ 9, s ~ Ó Ó _ C Ó$ í s BNdT [ j b _ ï À Óì õ ° ú y Ä »

o\ H % ò ¾ Ó` ¦ p 2 ; H כ ` ¦ r ô Ç . © s : r ¸_ þ j@ /° ú כ É r 632

C Ð Bi õ e ç ' ÷ &

· ú § É r BNdT r « Ñ\ " f ' a ¹ 1 Ï ÷ &% 3 Ü ¼ 9, © s : r ¸ H Bi ' | ¾ Ós 7 £ x < Ê\ " f 616

C t t 5

Å q& h Ü ¼ Ð ± ú & . s Qô Ç õ [ þ t ÐÂ Ò' 5 mol%_ Bi õ e ç ' BNdT [ j b r « Ñ_ l & h :

£ ¤$ í ¾ Ó © \ © Ä »o > 6 x H כ Ü ¼ Ð ó ø Íé ß ) a .

PACS numbers: 77.84.Cg, 77.80.-e, 77.22.-d, 68.55.jm, 68.55.Ln Keywords: [ j b Û ¼, q Û ¼Á ºÛ ¼ 8 £ x © ½ ¨ ¸, q Û ¼Á ºÛ ¼ õ e ç '

© Ä » ^ [ j b É r Z } É r Ä » : £ ¤$ í õ · ú : £ ¤$ í , Õ ª o

¦ y © Ä » : £ ¤$ í ` ¦ ° ú l M :ë H \ » ¡ ¤ l , q 6 fµ 1 Ï$ í B j ¸ o

Õ ªo ¦ G ' p" f 1 p x \ 6 £ x6 x| ¨ c Ã º e . : £ ¤ y , @ /³ ð& h y © Ä

» ^ Ó ü t| 9 Pb(Zr,Ti)O 3 (PZT)\ ¦ s 6 x ô Ç [ j b É r Ä

ºÃ ºô Ç y © Ä » $ í õ · ú $ í ` ¦ ? /# Q © \ O & h Ü ¼ Ð # Q ì

r \ s 6 x ÷ & ¦ e . Õ ª Q PZT_ â Ä º © s : r ¸ (T c ) 350 ^◦ C & ñ ¸ Ð, z ´F & h Ü ¼ Ð 150 ^◦ C s _ z ´ : r

â \ " fë ß è Ð s 6 x 0 p x . " f, þ j H ¦ : r ¨ 8

â

\ " f 1 l x H [ j b è \ ¦ > µ 1 Ï l 0 Aô Ç ½ ¨[ þ t s

' ÷ & ¦ e [1]. ¦ : r ¨ 8 â \ " f 6 x l 0 AK " f H Ó ü t

_ © s : r ¸ Z } H X <, y © Ä » ^ Ó ü t| 9 × æ q Û

¼Á ºÛ ¼ 8 £ x © ½ ¨ ¸\ ¦ t H Bi 4 Ti ₃ O ₁₂ (BIT) Ó ü t| 9 É r

É

r y © Ä » ^ Ó ü t| 9 \ q K © @ /& h Ü ¼ Ð Z } É r © s : r ¸

¦ t ¦ e .

Û ¼Á ºÛ ¼ 8 £ x © ½ ¨ ¸ y © Ä » ^ BIT H (Bi 2 O 2 ) ²⁺ (A m−1 B m O 3m+1 ) ²⁻ Ü ¼ Ð ³ ð & ³÷ & 9, A o

ü < B o \ y y Biü < Ti 0 Au K e ¦, q Û ¼Á ºÛ ¼ 8

x s \ 3> h_ ` ÐÚ ÔÛ ¼ s à Ô 8 £ x s Á ú ¢# e H ½ ¨ ¸

¦ s À Ò ¦ e . BIT [ j b É r PZT [ j b , KNN [ j b

Ð ± ú É r · ú , y © Ä » : £ ¤$ í ` ¦ Ðs l M :ë H \ La, Nd, Sm ° ú É r B ÐÀ Ó\ ¦ ' K " f : £ ¤$ í ` ¦ > h 9 H

¨ ´ ú §s ' ÷ & ¦ e [2]. Õ ª × æ \ " f Nd\ ¦ '

y © Ä » : £ ¤$ í õ Ä » : £ ¤$ í s a % ~ t H õ µ 1 Ï³ ð÷ &

3 [3]. Õ ª Q BIT> [ j b ` ¦ ] j l 0 AK " f H Z

} É r : r ¸\ " f è ` ¦ K ¦, s õ & ñ \ " f Ô ¦ î ß & ñ ô Ç Bi ~ 1 > 6 fµ 1 Ï÷ & H ë H ] j e [4]. Bi_ 6 fµ 1 Ï Ð K

ª s : r < Ês Ò q t$ í ÷ & ¦, s Qô Ç < Ê É r ì r F

G x Ð & ³ © ¢ ¸ H ¾ º[ O À Ó 1 p x` ¦ 7 £ x r & Ó ü t| 9 _ y © Ä

» : £ ¤$ í x 9 l & h : £ ¤$ í \ É r % ò ¾ Ó` ¦ p 2 ; .

f Bi\ ¦ õ e ç ' # Bi_ 6 fµ 1 Ï` ¦ Ð © #

< Ê` ¦ y èr & : £ ¤$ í ` ¦ > h r v H ½ ¨[ þ t s Ö ¸ µ 1 Ï >

' ÷ & ¦ e [5]. : r ½ ¨\ " f H l & h : £ ¤$ í s Ä ºÃ º ô

Ç ¸$ í ` ¦ % 3 l 0 AK BIT\ Nd\ ¦ ' ô Ç BNdT [ j b

\ Bi\ ¦ õ e ç ' # ¦ © ì ø Í6 £ xZ O Ü ¼ Ð ] j % i .

j ) a BNdT [ j b \ " f q Û ¼Á ºÛ ¼ 8 £ x © ` ÐÚ ÔÛ ¼ s à

Ô © + þ A$ í É r X- r] X (X-ray diffraction, XRD)` ¦ : x K

S X % i . Õ ªo ¦ Ä » © Ã º, Ä » < Hz ´, ï ß À Óì rF G Õ

ªo ¦ ½ Ó l © ` ¦ 8 £ ¤& ñ # Bi _ õ e ç ' | ¾ Ó\ É r T _c ü < l & h : £ ¤$ í x 9 y © Ä » : £ ¤$ í ` ¦ ¸ % i .

Bi 2 O 3 (99.9%, Sigma Aldrich), Nd 2 O 3 (99.9% Sigma Aldrich), TiO ₂ (99.9% Sigma Aldrich) ì r ´ ú ` ¦ " é ¶ « Ñ Ð ¦

© ì ø Í6 £ xZ O Ü ¼ Ð Bi\ ¦ õ e ç ' ô Ç BNdT [ j b ` ¦ ] j ¸

i . BNdT [ j b É r Bi 3.84 Nd 0.16 Ti 3 O 12 ¸$ í q Ð Bi\ ¦ 0 mol% \ " f 20 mol% t õ e ç ' % i . Bi õ e ç '

| ¾ Ó\ BNdT [ j b ` ¦ y y BNdT-0%, BNdT-5%, BNdT-10%, BNdT-15% Õ ªo ¦ BNdT-20%Ü ¼ Ð " î % i

. " é ¶ « Ñì r ´ ú õ \ ò ø Í` ¦ õ t Ø Ô ïm ^ ¦` ¦ [ O # Q 12r ç ß 1

x î ß 1 ^ ¦x 9 Ð D ¥ ½ + Ë % i ¦, 120 ^◦ C \ " f Ø æì r y | ¸

% i . | ¸ ) a ì r ´ ú ` ¦ · ú À Òp ¸m \ V , ¦ 740 ^◦ C

" f 2r ç ß 1 l x î ß 1 è % i . è ) a ì r ´ ú ` ¦ 0 A õ

ñ õ 1 l x{ 9 ô Ç ¸| Ü ¼ Ð 2 ^ ¦x 9 ` ¦ ¦ | ¸ô Ç Ê ê 2

è % i . 2 è = å Q è ß ì r ´ ú \ 5 wt% polyviny- lalcohol (PVA)\ ¦ D ¥ ½ + Ë # Ä »µ 1 Ï Ð ì r W # ^ è H ß ¼l

100 µm ^ Ð ^ 2 £ § % i . Õ ª + '\ 10 mm F K + þ

Ad ¦ \ " f · ú $ í + þ Aô Ç Ê ê 1100 ^◦ C \ " f 2r ç ß 1 l x î ß è

% i . è Ê ê r « Ñ[ þ t _ l & h : £ ¤$ í ` ¦ 8 £ ¤& ñ l 0

AK 500 µm Ð / B N ¦ É r (Ag) F G` ¦ 7 £ x Ã Ì % i .

X- r] X © u (XRD, RIGAKU MAX-2500)\ ¦ s 6 x K

f Bi 3.84 Nd 0.16 Ti 3 O 12 [ j b _ & ñ ½ ¨ ¸\ ¦ ì r$ 3 % i

Fig. 1. (Color online) XRD patterns of BNdT ceramics with different excess bismuth concentrations sintered at 1100 ^◦ C.

. Piezoelectric evaluation system (PES, aixACT aix- PES)` ¦ s 6 x # ô Ç l © \ É r y © Ä » s § 4 / B G

` ¦ 8 £ ¤& ñ % i ¦, e x ~ Û ¼ ì r$ 3 l (HP4194A)\ ¦ s 6 x

# 100 Hz - 10 MHz Å Ò Ã º # 3 0 A\ " f © : r Â Ò' 700

◦ C t Ä » © Ã ºü < Ä » < Hz ´` ¦ 8 £ ¤& ñ % i .

III. ÷ m Ç] M ö+ s ÇÊ Ý õ m Í w ² o

Figure 1 É r Bi ' | ¾ Ó\ É r BNdT-0%, BNdT-5%, BNdT-10%, BNdT-15% Õ ªo ¦ BNdT-20% [ j b _ X-