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JOURNAL OF APPLIED PHYSICS 99, 104101 共2006兲
a兲
Author to whom correspondence should be addressed; electronic mail: FIG. 1. Schematic diagram of the silver coplanar waveguide transmission
m.suherman@bham.ac.uk line patterned on the ferroelectric thin film and its MgO substrate.
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104101-2 Suherman et al. J. Appl. Phys. 99, 104101 共2006兲
TABLE I. Cell parameters of films deposited at various oxygen pressures and annealed in situ.
ef f = − 冉 冊
c 0␥
2 f
2
, 共1兲
given. The films grown at high pressure tended to be cubic at
room temperature, whereas the films grown at low pressure
tended to be tetragonal. For low pressure deposition, the out-
where c0 is the speed of light in a vacuum and f is the of-plane lattice parameters had greater expansion compared
measurement frequency. The real part of permittivity of the with the in-plane lattice parameter. The expanded out-of-
film 共 兲 was obtained from the conformal mapping method
⬘
for coplanar waveguide transmission lines,8 from which the
plane lattice parameter of films grown at low pressure may
be indicative of greater structural disorder or of increased
following result is obtained: oxygen vacancies.
1 EDX measurements showed that the composition of all
⬘ = 关共2⬘ef f 兲 − 共q2s兲 + q2 − 2 + 共q1s兲兴. 共2兲 the films grown at various pressures was consistent with the
q1
commercially nominal stoichiometry of the target to within
In Eq. 共2兲, s is the permittivity of the substrate 共assumed to an error of 0.5%.
be purely real, appropriate for a very low loss substrate such The cross-sectional TEM pictures revealed a columnar
as MgO兲, ⬘ef f is the real part of effective permittivity, and q1 structure for all in situ annealed films irrespective of deposi-
and q2 are geometrical factors involving the transmission line tion pressure, with a column width ⬃50 nm 关Fig. 2共a兲兴. EDX
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104101-3 Suherman et al. J. Appl. Phys. 99, 104101 共2006兲
FIG. 3. Magnitude of return loss 共兩S11兩兲 and phase shift 共arg S12兲 of a silver
coplanar waveguide on BST/MgO film deposited at 10−1 mbar and annealed
ex situ. Data is shown for electric field biases of 0 共solid line兲 and 3.2
共dashed line兲 V m−1.
In situ Ex situ
Annealing Annealing
FWHM 共°兲 0.8657 0.2654 FIG. 4. Real part of the permittivity of a film deposited at 10−1 mbar and
In-plane cell parameter 共Å兲 3.95896±0.00152 3.96033±0.00095 annealed ex situ. 50% tunability was obtained between 0 and 3.2 V m−1
Out-of-plane cell parameters 共Å兲 3.94851±0.00075 3.95549±0.00075 electric field bias. The dashed lines show the permittivity calculated from
the time domain measurement.
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104101-4 Suherman et al. J. Appl. Phys. 99, 104101 共2006兲
FIG. 5. Tunability 共䊊兲, effective dielectric loss tangent 共⫹兲, and permittivity
共䉭兲 of in situ annealed films deposited at various oxygen pressures. Data at
20 GHz and 1.6 V m−1 are shown.
FIG. 6. Comparison of the tunability of films annealed in situ and ex situ as
a function of electric bias field.
is metal thickness, ␦c is the skin depth, and s is half of the
center-width of CPW.10,11 For transmission lines 300 nm
thick, with s = 25 m, and conductivity = 3.7⫻ 107 S / m capacitance-voltage curve in low frequency studies. There
obtained from van der Pauw measurements, the frequency was no hysteresis at 300 K but hysteresis was observed at
limit is confirmed as f ⬎ 3 GHz. 80 K.
If the permittivity is assumed to be independent of fre- While films deposited at 10−1 mbar oxygen pressure did
quency, it can be determined directly from the propagation not show significant hysteresis at 300 K, films deposited at
delay for signals launched onto the transmission lines. This 10−1 mbar oxygen pressure showed pronounced hysteresis at
delay was obtained from time domain analysis of S12.12 The the same temperature. This suggested that films deposited at
real part of the effective dielectric permittivity was then cal- 10−1 mbar oxygen pressure were in the paraelectric state at
culated from Eq. 共4兲, room temperature while films deposited at 10−1 mbar oxygen
⬘ef f = − 冉 冊
c 0t l
l
2
, 共4兲
pressure were in the ferroelectric state despite the ex situ
annealing.
The temperature dependence of ⬘共E兲 of a film deposited
where tl and l are delay time and length of the transmission at 10−1 mbar and annealed ex situ are shown in detail in Fig.
line, respectively. The data calculated from this delay time 8. Figure 8 shows data for dc-bias voltages from 0 to 90 V.
was comparable with that derived previously, as shown in The permittivity shows a broad maximum at temperature
Fig. 4. Tmax which increases with bias voltage. This Tmax is not ex-
The permittivity of the films was strongly dependent on pected to be equal to Curie temperature Tc. In order to find
the oxygen pressure during deposition. Figure 5 shows the Tc, the inverse of real permittivity was plotted against tem-
real dielectric permittivity ⬘, tunability at 1.6 V m−1 and perature as shown in Fig. 9. Tc was found to be 225 K from
effective dielectric loss measured at 20 GHz for in situ an- the temperature intercept of the straight line fitted to data
nealed films. The tunability of the films is defined as above Tmax. This is in reasonable agreement with the value
⬘共V兲 − ⬘共0兲 expected for bulk material. The value of Tc was seen to de-
Tuneability = 100 % , 共5兲 crease with increasing bias voltage. A value for the Curie-
⬘共0兲
where ⬘共V兲 and ⬘共0兲 are real parts of the permittivity at
dc-bias voltage V and 0 Volts, respectively.
Films grown in an oxygen pressure of 10−1 mbar with
the other parameters set as described in Sec. II reproducibly
had the highest tunability. Films grown at 10−1 mbar had the
smallest cell parameters and tended to have a cubic structure
rather than tetragonal. This lower permittivity of in situ an-
nealed films deposited at lower oxygen pressure seems to be
due to the mechanical strain and oxygen defects.
After ex situ annealing, films deposited at 10−1 mbar did
not show any improvement in tunability. However, ex situ
annealing greatly increased the tunability of films deposited
at 10−4 mbar as shown in Fig. 6. The tunability was in-
creased by ⬃30% compared with the in situ annealed films.
FIG. 7. ⬘共E兲 curve of an ex situ annealed film deposited at 10−1 mbar
Figure 7 shows the ⬘共E兲 curve for measurement at 80 K
oxygen pressure. 䉱 and 쎲 represent the permittivity when voltage was
and 300 K of films fabricated at 10−1 mbar oxygen pressure swept up and down, respectively in order to demonstrate any hysteresis
and annealed ex situ. The ⬘共E兲 curve is equivalent to a behavior.
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104101-5 Suherman et al. J. Appl. Phys. 99, 104101 共2006兲
slope of the data in Fig. 9 according to Equation 共7兲 is frequently used to describe the behavior of
relaxor ferroelectrics measured at lower frequency
共100 Hz– 10 MHz兲 共Refs. 15–17兲 but the derivation does not
1 1 T − Tc require any particular frequency dependence. The parameter
= . 共6兲 , which quantifies the “diffuseness” of the transition, in-
⬘ 0 c
creases linearly with bias field. A similar increase in diffuse-
ness with bias was reported for Sr1−xBaxNb2O3.18 An increas-
This is in good agreement with values published ing suggests an increase in disorder within the sample, or
equivalently a widening of a distribution of Curie tempera-
elsewhere.13,14
ture or permittivity. Considering first the disorder, we might
Tmax was sensitive to the annealing process and oxygen
imagine that in zero-field bias, dipole moments are oriented
pressure during film fabrication 共Fig. 10兲. Films grown at the
in a direction other than parallel to the plane of the film. In
optimal 10−1 mbar showed a lower Tmax when annealed
these transmission line structures, the bias field is principally
ex situ compared with those annealed in situ. The highest parallel to the plane of the film. An increase in bias field will
Tmax was obtained for films grown at 10−1 mbar and reorient some of the dipoles and cause an increase of disor-
annealed in situ der. Considering a distribution of dielectric properties, we
The broad transitions to the ferroelectric state shown in might associate the regions with different permittivity as
Figs. 8 and 10 are indicative of heterogeneous films and inter- and intracolumnar regions.19 If the dependence of per-
therefore the dependences of Tmax and Tc on applied voltage mittivity on electric field is different in these two regions,
are not taken as indicative of the order of the ferroelectric- then the bias field will broaden the distribution of permittiv-
paraelectric phase transition. The solid lines in Figs. 8 and 10 ity within the whole sample. A third interpretation of the
are fits of Smolenski’s description17 of diffuse ferroelectric increase in is that the applied bias field increases the dis-
transitions, Eq. 共7兲, to the data, tribution of built-in electric field and strains generated by
charged defects.13,14 This will be considered in a later paper.
The effective loss tangent tan ␦ef f of the same film as in
Figs. 8 and 9 is shown as a function of temperature in Fig.
11. The peak in tan ␦ef f coincides with the peak in permittiv-
ity. The electric field bias lowers and broadens the peak in
tan ␦ef f so severely that it is impossible to say if the tempera-
ture of the peak moves significantly 共outside the error bars兲.
This tan ␦ef f contains contributions from both conductor 共␣c兲
and dielectric losses 共␣d兲. The conductor loss is linearly pro-
portional to the temperature dependent line resistance and
proportional to the square root of the line capacitance, which
involves the permittivity of the film, thus creating a distinct
peak in tan ␦ef f .
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104101-6 Suherman et al. J. Appl. Phys. 99, 104101 共2006兲
FIG. 12. 共a兲 Insertion loss and 共b兲 differential phase shift per unit length, for FIG. 14. Temperature dependent permittivity ⬘ 共쎲兲, tunability 共䉭兲, and
films deposited at various oxygen pressures. figure of merit 共⫹兲 for a film deposited at 10−1 mbar and annealed ex situ.
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104101-7 Suherman et al. J. Appl. Phys. 99, 104101 共2006兲
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