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Journal of Electromagnetic Waves and Applications

ISSN: (Print) (Online) Journal homepage: https://www.tandfonline.com/loi/tewa20

Dielectric characterisation and numerical


investigation of SrBi2Nb2O9–Bi2O3 composites for
applications in microwave range

R. F. Abreu , S. O. Saturno , J. P. C. do Nascimento , E. O. Sancho , J. E. V. de


Morais , J. C. Sales , D. X. Gouveia , H. D. de Andrade , I. S. Queiroz Júnior & A.
S. B. Sombra

To cite this article: R. F. Abreu , S. O. Saturno , J. P. C. do Nascimento , E. O. Sancho , J. E. V.


de Morais , J. C. Sales , D. X. Gouveia , H. D. de Andrade , I. S. Queiroz Júnior & A. S. B. Sombra
(2020) Dielectric characterisation and numerical investigation of SrBi2Nb2O9–Bi2O3 composites
for applications in microwave range, Journal of Electromagnetic Waves and Applications, 34:12,
1705-1718, DOI: 10.1080/09205071.2020.1787231

To link to this article: https://doi.org/10.1080/09205071.2020.1787231

Published online: 09 Jul 2020. Submit your article to this journal

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https://www.tandfonline.com/action/journalInformation?journalCode=tewa20
JOURNAL OF ELECTROMAGNETIC WAVES AND APPLICATIONS
2020, VOL. 34, NO. 12, 1705–1718
https://doi.org/10.1080/09205071.2020.1787231

Dielectric characterisation and numerical investigation of


SrBi2 Nb2 O9 –Bi2 O3 composites for applications in microwave
range
R. F. Abreu a,b , S. O. Saturnoa,b , J. P. C. do Nascimentob,c , E. O. Sanchod , J. E. V. de
Moraisb , J. C. Salesb,e , D. X. Gouveiab,c , H. D. de Andradef , I. S. Queiroz Júniorf and
A. S. B. Sombrab,f
a Telecommunication Engineering Department, Federal University of Ceará (UFC), Fortaleza, Brazil; b Physics
Department, LOCEM–Telecommunication and Materials Science and Engineering of Laboratory (LOCEM),
Federal University of Ceará (UFC), Fortaleza, Brazil; c Instituto Federal de Educação, Ciência e Tecnologia,
PPGET, Fortaleza, Ceará, Brazil; d Department of Mechanical Engineering, University of Fortaleza – UNIFOR,
Fortaleza, Brazil; e Departamento de Engenharia Civil, Centro de Ciências Exatas e Tecnologia, Universidade
Estadual do Vale do Acaraú, Sobral, Brazil; f Federal University of Semiarid Region, UFERSA, Mossoró, Brazil

ABSTRACT ARTICLE HISTORY


We present a study of the dielectric properties and behaviour of Received 29 December 2019
dielectric resonator antennas (DRAs) based on SrBi2 Nb2 O9 (SBN)- Accepted 19 June 2020
Bi2 O3 composites. X-ray diffraction is used for structural characteri- KEYWORDS
sation of the samples and it indicates the formation of a new phase SrBi2 Nb2 O9 ; microwaves;
after the addition of Bi2 O3 . The temperature coefficient of resonant solid-state reaction; dielectric
frequency (τ f ) is measured and the results demonstrate that the resonator antennas
increment of Bi2 O3 improves the thermal stability of the composites
from −345.62 to −235.02 ppm/°C. For the dielectric properties, it is
observed that Bi2 O3 additions cause the formation of new phases,
which present higher dielectric ε’ than SBN. Our numerical simula-
tions show that the materials operate as DRAs and that SBN-Bi2 O3
composites could be potential candidates for DRAs operating in the
S band.

1. Introduction
Recent progress in microwave telecommunications, satellite broadcasting and intelligent
transport systems has resulted in an increase in the demand for low loss dielectric res-
onators with dielectric properties capable of operating in the microwave range [1–6]. The
challenges surrounding communication systems technology involve research in various
areas of knowledge to meet the demands of the rapidly expanding consumer market. Thus,
it is necessary to constantly search for new materials that provide the improvement of
these and other technologies, with in-depth studies in the microwave area. In this context,

CONTACT R. F. Abreu roterdan.fernandes@gmail.com Telecommunication Engineering Department, Federal


University of Ceará (UFC), Fortaleza, Ceará 60755-640, Brazil; Physics Department, LOCEM–Telecommunication and
Materials Science and Engineering of Laboratory (LOCEM), Federal University of Ceará (UFC), Fortaleza, Ceará 60455-760,
Brazil

© 2020 Informa UK Limited, trading as Taylor & Francis Group


1706 R. F. ABREU ET AL.

dielectric ceramics have brought tremendous innovation to the microwave wireless com-
munications industry, reducing both the size and cost of electronic components, such as
filters, oscillators and antennas. Furthermore, these materials have high permittivity and
low losses, thereby presenting numerous applications from cellular to global positioning
systems [3,6].
Among ceramic materials, the bismuth layer ferroelectric group is a class of compounds
that is known for its fatigue strength and that has been extensively investigated due to its
potential use in random access memories. These oxides with the perovskite structure are
stable and have high permittivity values, good piezoelectric coefficients and spontaneous
polarisation. Therefore, they represent a class of materials suitable for use in many techno-
logical applications [7]. The matrix SrBi2 Nb2 O9 (SBN) is a perovskite with an orthorhombic
structure and space group (Laue group) A21 am that presents a high Curie temperature
(430°C). Due to its low sintering temperature, this ceramic is considered a low-temperature
co-fired ceramic material [8–12].
Therefore, the purpose of this work is to study the dielectric properties of the matrix SBN
with the addition of Bi2 O3 for microwave systems and applications. X-ray diffraction (XRD)
is used for the structural characterisation of the samples. The dielectric properties in the
microwave range are measured by the technique developed by Long, Macllister and Shen
[13,14], and through the Hakki–Coleman method [15,16]. The temperature coefficient of
resonant frequency (τ f ) is studied to determine the thermal stability of the material. Finally,
the behaviour of the composites as dielectric resonator antennas (DRAs) is investigated
through numerical simulations.

2. Experimental
2.1. Materials and structural analysis
Analytical grade SrCO3 (Aldrich, 99.9% purity), Bi2 O3 (Aldrich, 99.9% purity), and Nb2 O5
(Aldrich, 99.9%) were used to synthesise SBN through the solid-state reaction method
according to Equation (1). Reagents were inserted into a polyacetal container together with
zirconia spheres and milled for 8 h on a Fritsch Pulverisette 5 planetary mill to promote mix-
ing and breaking of the particles. After this procedure, powders were calcined at 900°C for
2 h with a heating rate of 5°C/min.

SrCO3 + Bi2 O3 + Nb2 O5 → SrBi2 Nb2 O9 + CO2 ↑ (1)

To obtain the composites, SBN and Bi2 O3 were homogenised in a mortar and Bi2 O3 was
added to SBN in 3%, 5%, 10% and 15% mass proportions. These samples were denominated
as SBN, SBN3, SBN5, SBN10 and SBN15, respectively, indicating the percentage of Bi2 O3
added. The DRAs were produced using 5% of glycerin as a binder, followed by compaction
with uniaxial pressure at 294 MPa. SBN was sintered at 900°C for 2 h, whereas the compos-
ites were sintered at 850°C for 2 h. This lower sintering temperature for the composite is
due to the low melting point of Bi2 O3 .
The structural properties of the sintered ceramic composites were analysed by XRD
patterns obtained at room temperature using a Panalytical XPert Pro MPD diffractometer
(Co-Kα line, 40 kV, 30 mA and λ = 1.788965 Å) and the Rietveld method was successfully
applied to determine the quantitative phase in the materials [17,18].
JOURNAL OF ELECTROMAGNETIC WAVES AND APPLICATIONS 1707

2.2. Resonator configuration


The dielectric properties were initially studied using the technique developed by Long,
Macllister and Shen [6,13,14], and using an Agilent N5230A vector network analyser. This
technique consists of exciting the samples under the DRA configuration (see Figure 1),
where a coaxial/feed probe is inserted below the ground plane and the part to be analysed
must be positioned next to the probe. The earth plane used is made of copper and has
dimensions of 35.5 cm × 30 cm × 2.14 mm. The probe is connected to the ground plane
through an SMA connector of 50  and has a length of 9.6 mm. The cylindrical DRA has
radius a, height h and height of probe d.
Therefore, the DRA subjected to this process will operate in HE11δ mode. According to the
literature [19,20], the resonant frequency and quality factor (Q) can be accurately calculated
through Equations (2) and (3), respectively:
 a  a 2 
6.324c
f(HE11δ ) = √ 0.27 + 0.36 + 0.02 (2)
2πa εr + 2 2h 2h

and
   2  
1.3 a −2.05 0.5 ha − 0.0125 ha
Q(HE11δ ) = 0.01007(εr ) · 1 + 100e (3)
h

The return loss and Smith chart were measured using the N5230A and compared by
numerical simulations. The presence of air gaps directly influences the bandwidth and
impedance matching in the experimental measurements [21–23]. Thus, these parameters

Figure 1. Setup for the DRA measurement.


1708 R. F. ABREU ET AL.

are inserted in the theoretical model so that the simulation has the closest possible condi-
tions to the experimental measurements [24]. Therefore, we used numerical simulations in
order to obtain both distant field parameters and to validate the experimental process.

2.3. Microwave dielectric properties


The values of the permittivity (ε r ), loss tangent (tan δ) and loaded quality factor (Q = 1/tan
δ) were obtained by means of the Hakki–Coleman method and using a Hewlett-Packard
HP8716ET network analyser. The device consisted of a dielectric cylinder with radius a and
height h placed between two parallel conducting plates, as represented in Figure 2.
The dielectric resonator must present a diameter to height ratio close to two to obtain
wide mode separation so that the electromagnetic mode TE011 is not disturbed by other
adjacent modes [3]. Thus, a 300C Courtney resonator system (Damaskos Inc.) was used to
capture the signals detected by the receiving antenna, which were then treated with Court-
ney software (Damaskos Inc.). Finally, the program analysed the characteristic spectrum of
the sample to determine the resonance modes.
The temperature coefficient of resonant frequencies τ f was analysed through the
Silva–Fernandes–Sombra method [25] using an Agilent network analyser 8719ET. This
parameter is very important since τ f indicates how much the resonant frequency changes
with temperature. Many applications in electronic devices, such as microwave resonators,
require τ f values close to zero [3]. Mathematically, τ f can be expressed by:

1 f
τf = · ·106 ppm ◦ C−1 (4)
f0 T

Figure 2. Schematic sketch of Courtney setup for measuring the dielectric constant under end shorted
condition.
JOURNAL OF ELECTROMAGNETIC WAVES AND APPLICATIONS 1709

where f is the variation of resonant frequency (GHz), T is the temperature range (°C) and
f 0 is the resonance frequency at the beginning of the process (GHz).

2.4. Numerical simulations


We carried out numerical simulations with the aim of validating the experimental setup,
through which it is possible to obtain the radiation pattern of the antenna and the far-field
parameters (directivity, gain, efficiency radiation and radiation diagram), and to confirm the
sensitivity of the results concerning air gaps. The resonant frequency obtained by Equation
(2) is related to a probe-less DRA, so using simulations we can study the effect that the probe
®
has on the resonant frequency described by this equation. Ansoft HFSS [26] software uses
the finite element method to simulate electromagnetic fields to validate the experimental
results and to obtain essential parameters for the analysis of the ceramic samples as DRAs.

3. Results and discussion


3.1. Structural analysis
The identification of the phases was performed by XRD, with the diffractogram peaks
indexed using the JCPDS international database records. As observed in Figure 3, all sam-
ples showed a predominance of the SBN phase (identified with JCPDS No. 82-280) [8–12].
The diffractograms of the SBN5 and SBN15 samples presented small amounts of the phase

Figure 3. XRD pattern of SBN added Bi2 O3 *(Sr0.6 Bi0.305 )2 Bi2 O7 and ♦Bi3 NbO7 .
1710 R. F. ABREU ET AL.

Figure 4. Diffractogram for (a) SBN, (b) SBN3, (c) SBN5, (d) SBN10, (e) SBN15 and Rietveld refinement,
respectively.

(Sr0.6 Bi0.305 )2 Bi2 O7 (JCPDS no. 73-923), whereas SBN10 presented Bi3 NbO7 (JCPDS no. 81-
582) as a secondary phase. The formation of phases of bismuth can bring benefits, such as
the decrease in the sintering temperature of the material [27,28].
Rietveld refinement was performed for all samples and the results are shown in Figure 4.
The low residual values between the observed and calculated diffraction patterns indicate
that the realised refinement is reliable. Table 1 presents the parameters R−p , Rwp and S,
JOURNAL OF ELECTROMAGNETIC WAVES AND APPLICATIONS 1711

Table 1. Parameters obtained from the Rietveld refinement of SBN samples.


Theoretical Apparent Relative
Sample R−P R−WP S density (g/cm3 ) density (g/cm3 ) density (%)
SBN 12.43 17.19 1.90 7.27 6.55 91.47
SBN3 15.95 20.41 1.46 7.27 6.90 94.91
SBN5 12.04 16.52 1.21 10.95 6.98 63.74
SBN10 13.74 18.08 1.34 8.39 6.82 81.28
SBN15 17.43 22.07 1.61 7.61 6.93 91.06

where it is possible to observe that the refinement was satisfactory, since the values of the
parameters were adequate.

3.2. Microwave dielectric properties


The dielectric properties εr , tan δ and Q were obtained by the Hakki–Coleman method and
are presented in Table 2. It is noteworthy that the addition of Bi2 O3 resulted in an enhance-
ment in ε r , which is interesting for device miniaturisation. The changes observed in the ε r
values can be justified by the fact that the (Sr0.6 Bi0.305 )2 Bi2 O7 and Bi3 NbO7 phases have a
greater εr than SBN [29,30]. These phases are present in the composites, as informed in the
XRD analysis.
Moreover, it is observed that the increment of Bi2 O3 addition caused a small decrease in
tan δ and this behaviour could be explained by the fact that (Sr0.6 Bi0.305 )2 Bi2 O7 and Bi3 NbO7
present tan δ values close to the SBN phase [29,30]. This result is interesting for microwave
applications, since the lower the value of the loss tangent, the lower the dissipation of the
energy of the antenna [27,31].
SBN15 presented the highest value of dielectric permittivity (ε r = 104.82) and the lowest
value of the loss tangent (tan δ = 3.24 × 10−2 ) among all analysed samples.
Regarding the τ f , it was observed that its value increased with the increment of the addi-
tion, demonstrating that Bi2 O3 improves the thermal stability of SBN. Therefore, we can
say that the addition caused the improvement of the three main properties required for a
DRA [3].

3.3. SBN-based DRAs


The distant field parameters are of great importance, since they provide data regarding
the operation of materials, such as DRAs. These parameters were obtained for all samples
®
through numerical simulations employing Ansoft HFSS software. Through the numerical

Table 2. Dielectric properties of SBN samples doped with Bi2 O3 through the Hakki–Coleman method.
Samples εr D (mm) H (mm) tan δ (10−2 ) Qd (GHz) τ f (ppm/°C)
SBN 28.6 17.78 8.96 3.24 0.135 −345.62
SBN3 86.18 15.27 8.54 2.40 0.115 −322.46
SBN5 75.56 15.59 8.74 2.67 0.108 −362.07
SBN10 60.64 16.13 8.86 2.64 0.119 −305.56
SBN15 104.82 15.02 7.88 1.86 0.142 −235.02
Note: ε r (dielectric permittivity), D (diameter), H (height), tan δ (loss tangent), Qd (quality factor) and τ f for all samples.
1712 R. F. ABREU ET AL.

simulations, it was possible to compare the experimental and simulated results for the res-
onant frequency, return loss, input impedance, Smith chart, radiation patterns and other
far-field parameters.
Thus, under the DRA configuration proposed by Long, Macllister and Shen, the resonant
frequencies were determined around the first HE11δ mode, which is the lower frequency
mode (dominant mode). For this mode, the resonant frequencies of the five samples agreed

Figure 5. The figure shows the return loss of the five samples: (a) SBN, (b) SBN3, (c) SBN5, (d) SBN10 and
(e) SBN15. In these figures, it is possible to notice that the experimental and simulated graphs are well
refined.
JOURNAL OF ELECTROMAGNETIC WAVES AND APPLICATIONS 1713

Table 3. Numerical and experimental processes for cylindrical DRAs.


f r (GHz) S11 (dB) BW (MHz)
Sample Exp. Simu. Exp. Simu. Error (%) Exp. Simu. Error (%)
SBN 2.86 2.86 −44.97 −45.01 0.08 120.62 103.75 13.90
SBN3 2.09 2.09 −63.93 −56.78 12.5 34.85 38.22 8.81
SBN5 2.14 2.13 −41.17 −41.19 0.04 41.88 46.35 9.64
SBN10 2.32 2.32 −50.98 −51.70 1.39 57.81 55.47 4.04
SBN15 2.00 2.00 −49.67 −48.03 3.41 30.47 32.01 4.81

with Equation (2). It is important to note that the increase of the addition of bismuth oxide
on the SBN matrix causes the growth in dielectric permittivity and, consequently, a decrease
in resonant frequencies for the HE11δ mode [20].
Figure 5(a–e) compares the experimental and simulated graphs for the return loss of
each sample. The simulated and experimental values for the resonance frequency and
return loss are in excellent agreement. In addition, it is observed that the return loss is
much lower than −10 dB, which means that less energy is returned to the source, i.e. more
energy is being transmitted. For wireless applications, the antenna operating frequency
band should have a return loss below −10 dB, corresponding to 10% reflected power
[29–32].
The results presented in Table 3 and Figure 5 show that the samples are operating as
DRAs. The error between the simulated resonant frequency and the measurement is practi-
cally 0%. For the value of S11 , the error is higher for SBN3 (12.50%), while the others samples
presented an error of less than 3.50%, as can be seen in Table 3. From Figure 5 and Table 3,
it is possible to observe a narrowing of the bandwidth of the DRAs with the addition. This
behaviour is explained by the fact that the composites present higher ε’ values than SBN.
The coupling between the transmission line and the antenna occurs by comparing
the simulated and experimental impedances. The analysis of this coupling was achieved
through the investigation of the complex impedance graphs and through the study of
the Z’() and Z"(). Figure 6 shows the experimental and simulated diagrams of the real
part of the Z’() and imaginary Z"(), where it is observed that the experimental and simu-
lated graphs have a good agreement. In addition, through the analysis of the impedances,
it is possible to notice that the additions contributed to the variation in the resonance
frequency of the antennas.
Figure 7 shows the experimental and simulated Smith charts of SBN and the composites.
Such a study becomes useful when it is necessary to express the character of the sample as
resistive, capacitive or inductive. In other words, the upper half of the graph above the hor-
izontal axis represents all positive impedances, i.e. inductive impedances, while the lower
half of the graph represents all negative impedances, i.e. capacitive impedances [33,34].
Figure 7(a–d) shows the loop of the experimental and simulated values shifted to positive
reactance, indicating that the samples have an inductive behaviour in the resonance, while
the other samples show a combination of inductive and capacitive reactance.
The paths in the respective inductive or capacitive semi-circular regions of the Smith
chart for all the samples cut the real axis exactly at 50 , promoting impedance matching
with the feed line. The results of the samples evidence the effectiveness of the method used
for the design of DRAs.
1714 R. F. ABREU ET AL.

Figure 6. In the figure, it is shown the diagram of the real impedance vs frequency, and imaginary
impedance vs frequency of the five samples: (a) SBN, (b) SBN3, (c) SBN5, (d) SBN10 and (e) SBN15.

Since the simulations on HFSS were adequate, it was possible to obtain far-field param-
eters (see Table 4), from which it is observed that the gain and efficiency of the composites
were lower than for the pure sample. Moreover, the addition of Bi2 O3 also resulted in a
decrease in bandwidth justified by the higher ε r of the composites [5,6].
Considering the results of far-field parameters and the omnidirectional character of the
materials, it is possible to verify that both the pure SBN and its composites with Bi2 O3 could
JOURNAL OF ELECTROMAGNETIC WAVES AND APPLICATIONS 1715

Figure 7. Experimental and simulated Smith Chart in HFSS for the five samples: (a) SBN, (b) SBN3, (c)
SBN5, (d) SBN10 and (e) SBN15.

be employed in the manufacture of radars and communication satellites operating in the S


band [33,34].
Figure 8 shows the simulated radiation pattern in the E θ plane, where = 0° and 90°
show that the symmetry of the lobes indicates a good coupling between the probe and the
sample indicated in the setup (Figure 1). The profile analysed shows a diagram typical of a
cylindrical DRA, where the maximum radiation is in θ = 0°. The other samples follow the
same profile.
1716 R. F. ABREU ET AL.

Table 4. Directivity, gain, experimental (Exp.) and simulated (Sim.), Bandwidth (BW) at −10 dB, input
power (Pin ), radiation power (Prad ), efficiency of conduction and dielectric (e) determined by simulations
in the HFSS.
BW (MHz)
Samples Directivity (dB) Gain (dB) Exp. Sim. Error (%) Pin (W) Prad (W) e (%)
SBN 6.62 5.56 120.62 103.75 13.90 0.99 0.78 78.19
SBN3 6.49 3.15 34.85 38.22 8.81 0.99 0.46 46.45
SBN5 6.26 2.85 41.88 46.35 9.64 0.99 0.45 45.74
SBN10 6.66 4.01 57.81 55.47 4.04 0.99 0.51 54.45
SBN15 6.90 3.11 30.47 32.01 4.81 0.99 0.41 41.85

Figure 8. Radiation diagram obtained through numerical simulation (HFSS) for sample SBN.

4. Conclusions
In this work, the effects of the addition of Bi2 O3 on the dielectric properties in the microwave
range and behaviour as DRAs of a SBN ceramic matrix have been investigated. The value
of τ f changed from −345.62 ppm/°C (SBN) to −235.02 ppm/°C (SBN15), indicating that the
increment of Bi2 O3 enhanced the thermostability of the material. Furthermore, the addition
caused the increase of ε r and the decrease of tan δ.
Through simulations using HFSS, SBN and its composites were evaluated as DRAs, where
it was possible to note that all the materials presented a reflection coefficient below −10 dB
and that the resonance frequency decreased with increasing Bi2 O3 , varying from 2.86
to 2.00 GHz. Moreover, it was observed that the gain, bandwidth and efficiency of the
composites were lower than for pure SBN.
According to the classification given by the IEEE and from the characteristics obtained
for SBN and its composites with Bi2 O3 , the composites presented could operate in the S
band and are potential candidates for use in communication satellites and radars.

Acknowledgments
This work was partly sponsored by the Brazilian Research Agencies CNPq (Conselho Nacional de
Desenvolvimento Científico e Tecnológico) (grant INCT NANO(BIO)SIMES), CAPES – Coordenação de
JOURNAL OF ELECTROMAGNETIC WAVES AND APPLICATIONS 1717

Aperfeiçoamento de Pessoal de Ensino Superior (grant PNPD), FINEP - Financiadora de Estudos e Pro-
jetos (grants INFRAPESQ-11 and INFRAPESQ-12) and the U.S. Air Force Office of Scientific Research
(AFOSR) (FA9550-16-1-0127).

Disclosure statement
No potential conflict of interest was reported by the author(s).

Funding
This work was partly sponsored by the Brazilian Research Agencies CNPq (Conselho Nacional de
Desenvolvimento Científico e Tecnológico) (grant INCT NANO(BIO)SIMES), CAPES – Coordenação
de Aperfeiçoamento de Pessoal de Ensino Superior (grant Project PNPD), FINEP – Financiadora de
Estudos e Projetos and the Air Force Office of Scientific Research [grant number FA9550-16-1-0127].

ORCID
R. F. Abreu http://orcid.org/0000-0001-8156-3910

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