Journal

J. Am. Ceram. Soc., 90 [2] 483489 (2007)

DOI: 10.1111/j.1551-2916.2006.01432.x
r 2006 The American Ceramic Society

Cation Ordering and Dielectric Characteristics in Barium Zinc Niobate

Chun-Te Lee,w Yi-Chang Lin, and Chi-Yuen Huang*
Department of Resources Engineering, National Cheng Kung University, Tainan 701, Taiwan

Che-Yi Su and Ching-Li Hu

R&D Technology Center, Yageo Corporation, Kaohsiung 811, Taiwan

required to reach a high-Q state, obtained a high Q value without observing a hexagonally ordered structure in a BZT
BaZrO3 system. Then, Davies and colleagues5,6 attributed the
improvement of the Q value to the segregation of Zr41 ion to the
boundary region to stabilize the grain boundaries. Likewise,
Chen et al.7 regarded the Q increase as a result of the decrease in
the lattice defects of grain boundary by examining the grain
growth at high sintering temperatures.
More recently, Reaney and colleagues8,9 observed that a prolonged soaking time below the temperature of orderdisorder
transition could enhance 1:2 ordering and lead to an increase of
the Q value. Janaswamy et al.10 showed that Ba(Mg1/3Ta2/3)O3
(BMT) could form an ordered trigonal phase or a disordered
cubic phase according to different preparation temperatures.
They reported that the ordering of Mg, Ta, and Nb cations is
clearly related to the ionic size, charge differences, and calcination temperature. As viewed from the literature, no information
exists regarding the effects of calcination condition on the degree
of 1:2 ordering and Q. Thus, this study aimed to investigate how
calcination and sintering conditions can affect the ordered structure and Q of a Ba(Zn1/3Nb2/3)O3 compound with Raman spectroscopy, X-ray diffractometry (XRD), and transmission
electron microscopy (TEM).

Barium zinc niobate (Ba(Zn1/3Nb2/3)O3) (BZN) complex perovskite has been reported to have special microwave dielectric
properties with close relation of its ordered structure. This study
investigated the effect of calcination on the evolution of ordered
structure and on quality factor with Raman spectroscopy, X-ray
diffractometry, and transmission electron microscopy. The results revealed that single calcination at a lower temperature inhibited the growth of the ordered domain during sintering. In
contrast, the 1:2-ordered domain in double-calcined BZN powder grew signicantly with a higher sintering temperature and a
longer soaking time. It is attributed that double calcination
caused a higher degree of 1:2 ordering and better homogeneity.
At the same time, the quality factor of the sintered ceramic body
was highly promoted when using double-calcined powder. A
close relation of the quality factor with the size of ordered domain, the degree of 1:2 ordering, and the relative density of BZN
ceramics was presented.

I. Introduction
complex perovskite compounds of Ba(B0 1/3B00 2/3)O3
(B 5 Mg21, Zn21; B00 5 Nb51, Ta51), which exhibit a
high relative permittivity, good quality factor (Q), and a nearzero temperature coefcient of resonant frequency (tf), have
been used in manufacturing dielectric resonators in the wireless
communication system. Previous researches have conrmed that
the barium zinc niobate (Ba(Zn1/3Nb2/3)O3) (BZN) ceramic had
excellent microwave dielectric properties, and the ordering of Bsite cations had a great effect on Q. Nevertheless, the extended
annealing time required for achieving a high-Q state slowed
down the commercialization of these ceramics, a shortcoming
that has drawn considerable attention since the 1980s.
Several researchers have discerned that the high-Q value results from cation ordering and can be achieved with annealing.
Firstly, Kawashima et al.1 reported that the Q value improved
with increasing degree of ordering, but with at least 120 h of
annealing to achieve a perfect hexagonal ordered structure.
Then, Endo et al.2 observed that the Q value increases with
the annealing temperature to reach a saturation value above
14001C.
By contrast, Desu and OBryan3 reported that improved Q of
Ba(Zn1/3Ta2/3)O3 (BZT) is observed even after the completion of
such an ordering. Thus, they implied that the improved Q value
was derived from the loss of ZnO at high temperatures or for
a long soaking time. Tamura et al.,4 who reported that minor
addition of BaZrO3 dramatically reduced the annealing time

HE
0

II. Experimental Procedure

Sample powders of BZN were prepared using a conventional
solid-state reaction method starting with BaCO3, ZnO, and
Nb2O5 (all of 99.9% purity), which were ball mill mixed in ethanol and with yttrium-stabilized zirconia media for 6 h. The
starting mix was heat treated with single and double calcination.
For single calcination, the dried mix was calcined at 10001C or
at 12501C, for 6 and 12 h in air, respectively. For double calcination, the starting mix was rst calcined at a low temperature
of 10001C for 6 h to remove CO2 and to avoid initial ZnO loss,
followed by a second calcination at 12501C for 12 h. After each
calcination, the calcined powders were all re-homogenized with
ball milling for 6 h. The green compacts were then sintered at
1250115501C for 448 h with both heating and cooling rates set
at 51C/min for sintering. The green compacts were sintered in a
crucible by mufing the BZN powder in order to reduce the
ZnO loss during sintering.
The phase composition was characterized using XRD (Siemens D5000, Bruker-AXS, Karlsruhe, Germany) with graphitemonochromated CuK1 radiation (l 5 1.5406 A) from 101 to
1201 2y, with a step size of 0.021 2y and a sampling time of 8 s/
step. The electron diffraction patterns of the polished samples
were obtained and analyzed using TEM (FEI Tecnai G2 F20,
FEI Philips, Eindhoven, the Netherlands;). Ramans spectra
were measured with a Dilor XY Raman spectrometer (J.Y.
Ramonor u1000 double monochromator, Horiba, Jobin Yvon
SAS, Longjumeau, France, 1 cm
1 resolution) with a detection
time of 10 s. Samples were excited by an Ar ion laser beam with
a wavelength of 515 nm and a power output of 100 mW.

P. Daviescontributing editor

Manuscript No. 21675. Received April 7, 2006; approved August 21, 2006.
Supported by the National Science Council of Taiwan under contract No.
NSC 94-2216-E-006-045.
*Member, American Ceramic Society.
w
Author to whom correspondence should be addressed. e-mail: C.T.Lee@yageo.com

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Journal of the American Ceramic SocietyLee et al.

The relative permittivity (er) and quality factor (Q) at microwave frequency (B6 GHz) were measured with the Hakki
Coleman dielectric resonator method using an HP 8757D network analyzer (Agilent Technologies, Palo Alto, CA) and an HP
8350B sweep oscillator (Agilent Technologies). The Q values
were determined using a TE011 resonant peak, and the temperature coefcient of resonant frequency (tf) was calculated after
measuring resonant frequency in the temperature range of 1251
to 1851C with
tf

f2
f1
;
f1 T2
T1

where f1 and f2 represent the resonant frequency at temperatures T1 and T2, respectively. To compare the dielectric characteristics at microwave frequencies, the product of quality factor
and resonant frequency (Q  f ) was used.

III. Results
(1) Phase Stability and Ordering: XRD Study
Figure 1 shows the XRD patterns of the powders calcined under
various conditions. All XRD patterns are indexed with the simple cubic perovskite structure. The pure BZN phase was formed
after 10001C/6 h of calcination. However, the single-calcined
powder of 12501C/12 h showed peaks of the second phase: barium niobate. Desu and OBryan3 proposed a mechanism to explain the formation of a ZnO-decient phase Ba3Ta2O8 in BZT
ceramic. In the current investigation, the second phase
Ba5Nb4O15 was conrmed from the data of energy-dispersive
spectroscopy (EDS) and the XRD pattern. It indicated that the
low synthesis temperature at 10001C effectively avoided initial
ZnO loss and removed CO2 to form the pure BZN phase.

Vol. 90, No. 2

The XRD patterns at a low angle were also investigated

(upper left inset of Fig. 1), and the weak superlattice reection
was found at 2y 5 B17.71. It is the formation of 1:2 ordered that
cause the trigonal symmetry P
3m1in unit cell. Moreover, the
weak superlattice reection of 1:1 ordering could be observed at
2y 5 B19.51 for the single-calcined powder at 10001C/6 h. It
shows that the 1:1 ordered Ba(Zn1/2Nb1/2)O3 phase was present
in this BZN powder. The intensity of the superlattice reections
is proportional to K fSfB0
fB00 g2 , where K represents a constant consisting of a polarization factor, a Lorentz factor, and
multiplicity factor; S is a long-range order parameter; and fB0
and fB00 are atomic scattering factors of B0 and B00 cations, respectively. The difference in scattering factor between Zn and
Nb ions is quite small, which leads to a much weaker intensity of
the superlattice reections than that of the fundamental reections.
On the other hand, the splitting of XRD peaks will occur
when ordering results in a lower symmetry. The (420) reection
at B114.61 2y will split into (422) and (226) reections in the
presence of 1:2 ordering. Proles of the (422) and (226) reections were examined at a high angle of XRD patterns under
different calcination conditions (upper right inset of Fig. 1).
However, no splitting of the (420) peak was observed, which
showed little lattice distortion in the BZN powders after any
calcination.
Noh et al.11 reported that the second phase, barium niobate,
was found when the BZN specimens were sintered at a temperature higher than 13501C. Figure 2 shows the XRD patterns
of sintered specimens with the double-calcined BZN powder (at
10001C/6 h and 12501C/12 h). No second phase was observed
when the sintering temperature was increased up to 14001C. It
appears that the second calcination at 12501C stabilized Zn in
the structure and reduced its vapor pressure during the nal
ring to prevent the formation of the second phase. However,
a prolonged soaking time at 13501C/48 h still caused the

Fig. 1. X-ray diffractometry (XRD) patterns of specimen calcined under various conditions. (a) Calcined at 10001C/6 h, (b) calcined at 12501C/12 h,
and (c) double-calcined at 10001C/6 h and 12501C/12 h.

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Dielectric Characteristics in Barium Zinc Niobate

485

Fig. 2. X-ray diffractometry (XRD) patterns of barium zinc niobate (Ba(Zn1/3Nb2/3)O3) (BZN) ceramics from powders double calcined at 10001C/6 h
and 12501C/12 h, and sintered at (a) 13001C/4 h, (b) 13501C/4 h, (c) 14001C/4 h, and (d) 13501C/48 h.

second-phase barium niobate to form on the specimen surface

due to ZnO loss, although specimens were mufed in the powder
of the same composition during sintering.
The trigonal distortion caused by the cation ordering can be
revealed by the departure
of the lattice parameter, c/a ratio,
p
from the ideal value of 3=2 1:224745 in cubic symmetry.
Desu and OBryan3 reported that an improvement of the Q
value in BZT was accompanied by an increase in the c/a ratio
and the splitting of (420) into (422) and (226) reections with the
soaking time. In this study, the c/a ratio was held with little
change around 1.22471.2253 under 1300114001C sintering
conditions. Nevertheless, Fig. 2 revealed that a long soaking
time did cause the splitting of (420) into (422) and (226) reections at B114.61 2y (upper right inset of Fig. 2). This indicated
that 1:2 ordering was enhanced with longer soaking time from 4
to 48 h at 13501C. In contrast, the superlattice reection at
B17.71 2y disappeared, and the splitting of (420) reection was
not observed at 14001C, showing that the 1:2 ordering decreased
at 14001C. From the above XRD analysis, the orderdisorder
phase transition occurred at 14001C in these BZN specimens.

(2) Ordering-Induced Microstructures: TEM Study

Figure 3 shows the TEM analysis of the BZN specimen, double
calcined and sintered at 13501C/4 h. Figure 3(a) showed that one
grain consisted of several domains, which were separated by
anti-phase boundaries (APBs). The APBs were observed because of the inuence of chemical ordering regions, which had

nucleated out of phase. The APBs are easily distinguished because that they do not lie on a specific set of crystallographic
planes, whereas the ferroelastic domains have domain walls parallel to certain crystallographic planes.12 The presence of superlattice reections by chemical ordering could be veried from
selected-area electron diffraction (SAED) patterns. Figure 3(b)
shows the typical SAED pattern of the chemical ordering domains besides APBs, and it was indexed on the basis of a simple
cubic perovskite structure. The occurrence of 71/3{111}-type
superlattice reections clearly showed the presence of a 1:2 cation-ordered structure with a trigonal P
3m1 ) symmetry. Figure
3(c) shows the high-resolution TEM (HR-TEM) image of a 1:2
ordered domain in the BZN compound. The wavelength of the
superlattice modulation was 0.71 nm, which corresponded to the
triple of the {111}-planer spacing of simple cubic unit cell
(d111 5 2.363 A). It appeared that the B-site cations were arranged along the /111S direction as ZnNbNbZnNbNb
y in the BZN compound. It was difcult to distinguish the degree variation of 1:2 ordering by the SAED patterns. However,
the 71/3 {111} type of superlattice reections weakened and
diffused for the specimen sintered at 14001C, which indicates
that the degree of 1:2 ordering decreased because of the presence
of diffused superlattice reections in the SAED pattern. This
result was consistent with the observation of XRD patterns in
Fig. 2, in which superlattice reection at 2y 5 17.71 disappeared
to indicate an orderdisorder phase transition at 14001C.
Figure 4 shows the dark-eld image and the SAED patterns
using one set of 71/3 {111} reections to investigate the

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Journal of the American Ceramic SocietyLee et al.

(a)

(a)

(b)

APB

200 nm

(c)

200 nm

011

111

(b)

110

111

000

000

100

001
(d)

(c)

0.71nm

Fig. 3. Transmission electron microscopy (TEM) analysis of 1:2 ordering structure in barium zinc niobate (Ba(Zn1/3Nb2/3)O3) (BZN) sintered
at 13501C/4 h from double calcined powders. (a) Anti-phase boundaries
 
(APBs), (b) selected-area electron diffraction (SAED) pattern of 
110
zone axis, and (c) high resolution (HR-TEM) image.

sintered BZN specimen after being single calcined at 10001C/6 h.

The TEM dark-eld image (Fig. 4(a)) of the 13501C/4 h sintered
sample showed many small-ordered domains (regions of light
contrast), typically 2050 nm in size. Figure 4(b) shows that no
superlattice reections were observed in some dark regions of
Fig. 4(a). It appeared that the disordered structure existed in
these dark regions. Furthermore, Fig. 4(c) shows the existence of
1:1 ordered phase Ba(Zn1/2Nb1/2)O3 in the microstructure. It
appeared that the 1:2 ordered, the 1:1 ordered, and the disordered phase coexisted in the specimen. Figure 4(d) shows that
the ordered domain size did not grow signicantly on prolonging the soaking time from 4 to 48 h. It appeared that the growth
of ordered domains was restrained when the BZN powder was
single calcined at a low temperature (10001C/6 h).
Figure 5 shows a dark-eld TEM micrograph for the sintered
specimen of double-calcined BZN powder (at 10001C/6 h and
12501C/12 h). The dark regions did not correspond to the disordered regions but rather to the ordered domains whose super
lattice reections were not enclosed by the objective aperture of
TEM. Figure 5(a) shows that ordered domains, typically 50100

Fig. 4. Transmission electron microscopy (TEM) analysis of sintered

specimens after single calcination at 10001C/6 h. (a) Dark-eld image of
a specimen sintered at 13501C/4 h, (b) selected-area electron diffraction
(SAED) pattern of the disordered phase, (c) SAED pattern of the 1:1
ordered phase, and (d) dark-eld image of a specimen sintered at
13501C/48 h.

nm in size, were present in the specimen of a shorter soaking

time (4 h). The ordered domains grew by an order of magnitude
when the soaking time was increased from 4 to 48 h at 13501C,
as shown in Fig. 5(b) of lower magnication. Apparently, the
synthesis condition had a pronounced effect on the growth of
ordered domain in the sintered BZN specimen after comparing
Figs. (4) and (5).

(3) Analysis of Raman Spectrum

Kim et al.13 demonstrated that Raman spectroscopy is a useful
tool for probing the 1:2 ordering in Ba(Ni1/3Nb2/3)O3 and
Ba(Zn1/3Nb2/3)O3 compounds. If the B0 and B00 ions are randomly distributed, the structure is a disordered cubic perovskite
with Pm3m symmetry and there is no Raman-active mode present. For the 1:1 ordered structure of Fm3m symmetry, the Raman spectra will show four strong active modes at 105 cm
1 of
F2g(Ba), 378 cm
1 of F2g(O), 429 cm
1 of Eg(O), and 783 cm
1
of A1g(O). In addition to these four active modes, the Raman
spectra of the 1:2 ordered structure of trigonal P
3m1 symmetry
will show three extra active modes, 175 cm
1 of Eg(O), 269 cm
1
of Eg(Nb), and 294 cm
1 of A1g(Nb).
Figure 6(a) shows the Raman spectra of BZN powders calcined under different conditions. The spectra in this research
concurred with those in previous BZN studies,13,14 and the spectra of the 1:2 ordered trigonal P
3m1 structure are similar to
those of other complex perovskite compounds, such as

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Dielectric Characteristics in Barium Zinc Niobate

487

Fig. 5. Dark-eld transmission electron microscopy (TEM) images of the barium zinc niobate (Ba(Zn1/3Nb2/3)O3) (BZN) specimen after double
calcination and sintering at (a) 13501C/4 h and (b) 13501C/48 h.

BMT,15,16 BZT,17 and Ba(Mg1/3Nb2/3)O3.16,18,19 The 1:2 ordering showed up in BZN powders after different calcination conditions, which was evidenced from the extra weaker modes in
the close-up region in Fig. 6(a). It is also observed in Fig. 6(a)
that the stretch mode of the oxygen octahedra A1g(O) at 782
cm
1 shifted toward a higher wave number (786 cm
1) with
higher calcination temperature or double calcination, which implied a stronger bonding in the structure, and consequently a
more stable-ordered phase. Furthermore, the intensity of double

Fig. 6. (a) Raman spectra of barium zinc niobate (Ba(Zn1/3Nb2/3)O3)

(BZN) compounds calcined under different conditions. (b) Variation of
full width at half-maximum (FWHM) of four active modes under different calcination conditions.

calcination became clearly higher, indicating that the degree of

ordering was enhanced.
Figure 6(b) shows the variation of the full-width at half-maximum (FWHM) of four active modes in the Raman spectra
(Fig. 6(a)) under different calcination conditions. All FWHMs
of these active modes decreased with higher calcination temperature or double calcination, which suggested less variation in
the NbO bond length, and a higher degree of ordering.
Figure 7 shows the Raman spectra of the BZN specimens,
which were double calcined and sintered at different temperatures. The intensity of Raman-active modes increased with higher sintering temperature (from 13001 to 13501C), and with a
longer soaking time (from 4 to 48 h at 13501C), which suggested
that the 1:2 ordered nano-regions grew with sintering temperature and soaking time. Some weak peaks between 312 and 336
cm
1 were observed for the 13501C/48 h spectrum (Fig. 7(c)),
probably due to the formation of the second phase, barium niobate, from ZnO loss during sintering. For the 14001C/4 h spectrum (Fig. 7(d)), the intensity of all active modes decreased and
the width broadened, accompanied by the disappearance of the
active modes of the 1:2 ordering at 270 cm
1 of Eg(Nb) and 297
cm
1 of A1g(Nb). Apparently, the degree of ordering decreased

Fig. 7. Raman spectra of barium zinc niobate (Ba(Zn1/3Nb2/3)O3)

(BZN) ceramics that were double calcined and sintered at (a) 13001C/
4 h, (b) 13501C/4 h, (c) 13501C/48 h, and (d) 14001C/4 h.

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Table I. Microwave Dielectric Properties of BZN Ceramics Under Different Calcination and Sintering Conditions
Calcination condition

Sintering condition

10001C/6 h

12501C/4 h
13001C/4 h
13501C/4 h
13501C/48 h
13501C/4 hw
13501C/4 h
14501C/4 h
15501C/4 h
13001C/4 h
13501C/4 h
14001C/4 h
13501C/48 h
13501C/48 hz

12501C/12 h
10001C/6 h and 12501C/12 h
Double calcination

Relative density (%)

Second phase

er

Q  f (GHz)

97.2
97.6
97.8
96.2
97.5
85.5
96.5
93.8
96.7
96.4
95.4
95.0
93.8

None
None
None
Ba5Nb4O15
None
Ba5Nb4O15
Ba5Nb4O15
Ba5Nb4O15
None
None
None
Ba5Nb4O15
Ba5Nb4O15

39.4
40.9
40.2
39.2
40.1
35.3
39.9
38.2
40.6
39.4
41.1
39.7
37.7

5749
7094
8915
11 560
3720
9027
66 278
41 639
47 101
112 286
69 675
236 753
67 714

Annealing at 12501C/12 h after sintering of 13501C/4 h. zWithout mufing powder during sintering. BZN, barium zinc niobate (Ba(Zn1/3Nb2/3)O3).

and the orderdisorder transformation occurred after 14001C/4

h sintering. The orderdisorder transition temperature of BZN
is clearly lower than that of the BZT compound, which was
reported to be 16001C.20,21

(4) Microwave Dielectric Properties

Table I summarizes the microwave dielectric properties of BZN
ceramics under various calcination and sintering conditions. The
relative permittivity varies little around 3541, but the Q  f
values were signicantly affected by the calcination and sintering
condition.
For BZN specimens single calcined at 10001C/6 h and sintered for 4 h, there was no second phase formation, and all had a
high relative density (497%) but relatively low Q  f values. A
higher sintering temperature (1250113501C) did increase the
Q  f value but not by much. Prolonged soaking time (13501C/
48 h) also increased the Q  f value slightly. For sintered BZN
specimens after 12501C/12 h of single calcination, the relative
density decreased due to second phase formation, but the Q  f
value increased markedly.
For specimens double calcined at 10001C/6 h and 12501C/12
h, the Q  f values became much higher than those with single
calcination. The highest Q  f of 236,753 GHz was observed for
the specimen sintered at 13501C/48 h. Raising the sintering temperature (1300113501C) or prolonging the soaking time can increase the Q  f value, but not when sintered at 14001C or
without powder mufing during sintering to prevent ZnO loss.

On the other hand, the sintered BZN ceramics from doublecalcined powders showed much higher Q  f values. The homogeneity in BZN powders brought about by double calcination
caused a relatively high degree of 1:2 ordering in the structure as
evidenced by the analysis of XRD patterns and Raman spectra.
The ordered domains grew signicantly in this homogeneous
structure during sintering and resulted in high Q  f values. The
ordered domains in a 13501C sintered specimen grew by an
order of magnitude (from 100 nm to 1 mm) when the soaking
time was increased from 4 to 48 h, and this BZN ceramic showed
a high Q  f value of 236 753 GHz. However, prolonged sintering caused ZnO loss when powder mufing was not applied,
resulting in a lower density and a large reduction of the Q  f
value (to 67 714 GHz). Also, the orderdisorder phase transition
of BZN occurred at B14001C, and sintering at 14001C/4 h
caused a low degree of ordering and a decrease in the Q  f
value from 112 686 (13501C/4 h) to 69 975 GHz.

V. Conclusion
By examining the effects of calcination condition on the ordered
structure and the quality factor for BZN microwave dielectric
ceramics, this study has veried that the calcination condition
plays an important role in the formation of an ordered phase
and the growth of an ordered domain. The quality factor is
closely related to the size of ordered domain, the degree of 1:2
ordering, and relative density. A BZN specimen sintered at
13501C/48 h from the double-calcined powder possessed an er
of 39.7, a tf of 15 ppm/1C, and a Q  f value of 236 753 GHz.

IV. Discussion
This study shows that the calcination condition had a significant
inuence on the formation of 1:2 ordering and the growth of
ordered domain, which is closely related to the quality factor
(Q  f ). All BZN-sintered specimens from 10001C/6 h singlecalcined powders showed much lower Q  f values (372011 560
GHz) even when the sintering temperature or the soaking time
was increased. The low Q  f value was due to small ordered
domains (2050 nm) and a high density of APBs in the structure,
which was attributed to the poor homogeneity in the single-calcined powder. Furthermore, the low calcination temperature of
10001C caused a low degree of 1:2 ordering, and the formation
of the 1:1 ordered Ba(Zn1/2Nb1/2)O3 phase and a disordered
phase. The disordered phase is a Nb51-rich phase that was
formed in order to maintain the electroneutrality in the structure
by compensating the charge imbalance in the unstable Ba(Zn1/
2Nb1/2)O3 phase. The strong internal eld brought by from the
combination of these two charge-imbalanced phases would
inhibit the growth of ordered domains during sintering,14 and
resulted in low Q  f values.

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