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Temperature Dependence of the Permittivity and Loss Tangent of High-

Permittivity Materials at Terahertz Frequencies

Article  in  IEEE Transactions on Microwave Theory and Techniques · May 2005

DOI: 10.1109/TMTT.2005.845752 · Source: IEEE Xplore

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1266 IEEE TRANSACTIONS ON MICROWAVE THEORY AND TECHNIQUES, VOL. 53, NO. 4, APRIL 2005
Temperature Dependence of the Permittivity and
Loss Tangent of High-Permittivity Materials
at Terahertz Frequencies
Klaus Berdel, Student Member, IEEE, Jaime Gómez Rivas, Peter Haring Bolívar, Member, IEEE,
Peter de Maagt, Senior Member, IEEE, and Heinrich Kurz
Abstract—An analysis including the temperature depen-
dence of the permittivity and loss tangent of three low-cost and
high-permittivity materials (zirconium–tin–titanate, alumina, and
titanium–dioxide) in the terahertz frequency range is presented.
Such dielectric materials find varied applications in microwave
and terahertz systems and components. Their effective use under
varying environmental conditions or in space applications requires
a detailed knowledge about temperature dependencies. Here, mea-
surements using broad-band terahertz time-domain spectroscopy
are presented in the temperature range from 10 to 323 K. It is
shown that zirconium–tin–titanate and alumina provide a good
thermal stability of the permittivity, whereas the permittivity of ti-
tanium–dioxide exhibits a strong dependence on the temperature.
Index Terms—Ceramics, dielectric materials, dielectric thermal
factors, measurement, submillimeter waves, titanium compounds.
I. INTRODUCTION
D IELECTRICS that combine high permittivity with low
losses are commonly used in microwave devices such as
waveguides, capacitors, antenna substrates, and electromagnetic
bandgap structures [1]–[3]. A critical parameter for the design
and performance of any device is the temperature dependence of
the permittivity and losses of the materials involved. In general,
a minimal temperature dependence is preferred, as devices made
of dielectrics with a strong temperature-dependent permittivity
have an undesirable variable performance under standard envi-
ronmental conditions. On the other hand, if the temperature can
be changed in a controlled and accurate way, the varying per-
mittivity can be used to the benefit of tunable devices [4]–[6].
Terahertz radiation comprises the part of the electromagnetic
spectrum lying between microwaves and infrared frequencies. A
great number of applications for this frequency range has been
identified [1]. However, due to the complexity and cost of cur-
rent technologies, terahertz has only been widely adopted in the
fields of astronomy and remote earth sensing [7]. This situation
Manuscript received May 19, 2004; revised July 6, 2004. This work
was supported by the Deutsche-Forschungsgemeinschaft and the European
Commission.
K. Berdel, J. Gómez Rivas, and H. Kurz are with the Institut für Halbleit-
ertechnik, Rheinisch Westfaelische Technische Hochschule Aachen, D-52056
Aachen, Germany.
P. Haring Bolívar was with the Institut für Halbleitertechnik, Rheinisch West-
faelische Technische Hochschule Aachen, D-52056 Aachen, Germany. He is
now with the Institute of High Frequency and Quantum Electronics, University
of Siegen, D-57068 Siegen, Germany.
P. de Maagt is with the Electromagnetics Division, European Space Research
and Technology Centre, 2201 AG Noordwijk, The Netherlands.
Digital Object Identifier 10.1109/TMTT.2005.845752
0018-9480/$20.00 © 2005 IEEE
changed with the advent of short-pulse lasers in the early 1990s,
which lead to the development of more flexibly and broadly us-
able terahertz systems. Terahertz technology is on the verge of
more widespread use. However, intense research is still neces-
sary to enhance the performance and efficiency of current tera-
hertz systems. One of the problems of terahertz technology is
the limited availability of precise information of electromag-
netic properties of materials in this frequency range.
In this paper, we present measurements in the terahertz
frequency range of the permittivity and loss tangent of three
materials, i.e., alumina Al O , zirconium–tin–titanate
Zr Sn TiO , and titanium–dioxide TiO at different
temperatures. These materials exhibit high permittivity and
low losses at room temperature [8]. They are cheap, easy to
process, and nontoxic. These materials are, therefore, also
good candidates for components and systems operating in the
terahertz frequency range.
The measurements have been performed in a broad-band
spectral range using a terahertz time-domain spectrometer.
Our measurements were carried out in the temperature range
from 173 to 323 K at intervals of 25 K. This range is wide
enough for most applications on earth. It also covers the typical
temperature variation of satellites in a geo-stationary orbit.
Therefore, the measurements presented here clear up the way
for the accurate development of terahertz devices for space
applications. Additionally, we also obtained the permittivity
and loss tangent at the lowest temperature that we could reach
in our setup, i.e., 10 K. This temperature is representative for
satellite missions into deep space.
II. TERAHERTZ TIME-DOMAIN SPECTROSCOPY
Terahertz time-domain spectroscopy uses short broad-band
terahertz pulses that are transmitted through the sample and de-
tected in the time domain. In order to generate and detect tera-
hertz radiation, the train of pulses of a femtosecond Ti : sapphire
laser is split in two. One of the beams is used to generate the
radiation by creating electron–hole pairs on the surface of an
InGaAs layer. The large surface field caused by the semicon-
ductor depletion layer accelerates these carriers, which act as
electric dipoles that emit terahertz pulses. The electromagnetic
field of these pulses is determined by the relation
, where is the current density of the accelerated
particles. After interacting with the sample under investigation,
these terahertz pulses are detected by a photoconductive switch
BERDEL et al.: TEMPERATURE DEPENDENCE OF PERMITTIVITY AND LOSS TANGENT OF HIGH-PERMITTIVITY MATERIALS
Fig. 1. (a) Terahertz transients. Black line: Reference pulse, measured
without sample. Dashed line: Pulse transmitted through a piece of alumina
with a thickness of 638 m at room temperature. (b) Terahertz spectra of the
reference signal and the transmission through the alumina piece. These spectra
are obtained by Fourier transforming the time-domain signals.
that is activated by the second laser beam. The photoconductive
switch consists of a metallic dipole antenna on a small piece of a
low-temperature grown gallium–arsenide (LT GaAs) with a sub-
picosecond carrier lifetime. The laser pulse generates carriers
on the LT GaAs that are driven by the terahertz electromagnetic
field producing a measurable current. This current is propor-
tional to the terahertz field amplitude during the carrier lifetime.
By varying the path length difference between the Ti : sapphire
beam used to generate the terahertz radiation and the beam em-
ployed to activate the switch, the time-dependent electric-field
transient is detected with subpicosecond resolution [9], [10].
The investigated samples were placed in a closed cycle cryo-
stat (CTI-cryogenics 8200), in which the temperature can be
easily varied and controlled from 323 K down to 10 K. Two
separate measurements have to be done in order to determine
the complex permittivity of a sample, i.e., a reference measure-
ment is taken through the cryostat, but without the sample to ob-
tain the response of the setup , and the second measure-
ment is the transmission through the sample . Typ-
ical terahertz transients are plotted in Fig. 1(a), where the solid
line represents the reference terahertz transient and the dashed
line is the transmission at room temperature through a piece of
alumina with a thickness of 638 m. The spectra and
are obtained by Fourier transforming the transients.
In Fig. 1(b), we present the spectrum of the reference signal with
1267
a solid line and that of the transmission through the alumina
piece with a dashed line. As can be appreciated in Fig. 1(b), the
spectral range of our setup extends from 0.25 to 4 THz, allowing
very broad-band measurements.
A fraction of the electromagnetic wave is always reflected at
an interface. The detected signal consists of the directly trans-
mitted pulse, as well as the multiple reflections at the samples
interfaces. The large thickness of our samples allows to distin-
guish these reflections from the directly transmitted pulse be-
cause they are separated in the time domain by a few picosec-
onds. Therefore, it is possible to filter the reflections in the mea-
surements and to omit them in the calculation of the sample
transmittivity. With this consideration, the transmitted ampli-
tude of a plane wave incident on a layer of the thickness
is given by
(1)
where is the complex refractive index of the sample, is
the speed of light in vacuum, and and
are Fresnel transmission coefficients of
the air–sample and of the sample–air interfaces, respectively.
If we write the complex refractive index as
, and we replace the Fresnel transmission coefficients into
(1), we obtain
(2)
where is the absorption coefficient.
Solving (2) numerically allows to determine the complex re-
fractive index from the measurements [11], [12]. The complex
permittivity and the loss tangent can be obtained
from
(3)
III. EXPERIMENTAL RESULTS
We have performed five measurements at each temperature,
illuminating different parts of the samples in each of these mea-
surements, in order to reduce the noise and to test the homo-
geneity of the samples. The permittivity and are the av-
erages of these five measurements. Besides the standard devia-
tion resulting from the different measurements, there are three
main sources of systematic error that also contribute to the un-
certainty of and , i.e., the thickness of the sample, the
focusing of the terahertz beam, and the scattering of terahertz
radiation.
Inaccuracies regarding the sample thickness affect the result
of the numerical solution of (2). Therefore, this thickness must
be accurately determined. We used a micrometer gauge with a
precision of 2 m to determine the sample thickness. This un-
certainty in the thickness induces a maximum error on of
1%, and of 0.5% in the loss tangent. Due to the thermal ex-
pansion of the samples, their thickness depends on temperature.
1268 IEEE TRANSACTIONS ON MICROWAVE THEORY AND TECHNIQUES, VOL. 53, NO. 4, APRIL 2005
Fig. 2. Terahertz pulses transmitted through a piece of titanium–dioxide with
a thickness of 1000 m measured at three different temperatures. Gray solid
line: transient measured at 323 K. Dotted line: measurement at 173 K. Black
solid line: measurement at 10 K.
Fig. 3. (a) Permittivity and (b) loss tangent versus the frequency of
titanium–dioxide given at different temperatures. Characteristic error bars are
indicated on the data measured at 10 K (solid gray).
Since we cannot determine the thickness of the samples while
they were mounted inside the cryostat, we estimated it from the
thermal expansion coefficient [13]. Thus, we found a variation
of the thickness for the three samples in the measured tempera-
ture range of less than 0.5%, which has a negligible effect on
and . The numerical solution of (2) assumes a plane wave
impinging on the sample at normal incidence. In our measure-
ments, the beam is focused onto the sample with an aperture
angle of 7 . At this maximum angle of incidence, the reflec-
tivity at the surface of the sample differs by less than 2% from
the one at normal incidence [14].
Equation (2) describes the coherent or forward scattered
transmission of the incident radiation [15]. The three samples
are opaque to the eye, which reveals the strong scattering at
Fig. 4. (a) Permittivity versus temperature for titanium–dioxide at 500 GHz,
(b) zirconium–tin–titanate at 500 GHz, and (c) alumina at 1 THz in the range
from 173 to 323 K. The circles are the measured data points. The lines represent
a fit of (4) to these measurements from which the temperature coefficient is
obtained of the permittivity.
optical frequencies due to inhomogeneities at length scales of
the order of the wavelength of light, i.e., 1 m. Scattering
generates a diffuse transmission at the expense of the coherent
transmission [16]. To properly account for scattering effects,
the diffuse transmission has to be measured by collecting it in
all directions with an integrating sphere [17]. Due to the limited
space inside the cryostat, it was not possible to perform this
measurement. Another possibility to investigate the effect of
scattering on the transmission could be to measure samples with
different thickness or with different sized particles. However,
the scattering is expected to be weak at terahertz frequencies
due to the large wavelength of this radiation compared with
the size of the inhomogeneities, and the consequent small
scattering cross section of the inhomogeneities. Therefore, we
may assume that scattering is negligible in the investigated
frequency range.
A. Titanium–Dioxide
The titanium–dioxide sample has a thickness of
m. The transmission measurements at three different temper-
atures are represented in Fig. 2, where the black, dashed, and
gray lines correspond to 10, 173, and 323 K, respectively. As
can be appreciated in Fig. 2, when the temperature is reduced,
the time delay of the transmitted pulse significantly increases.
This increase is due to the reduction of the group velocity of the
terahertz pulse, which is a consequence of the increase of the
BERDEL et al.: TEMPERATURE DEPENDENCE OF PERMITTIVITY AND LOSS TANGENT OF HIGH-PERMITTIVITY MATERIALS 1269

TABLE I
TEMPERATURE COEFFICIENT OF THE PERMITTIVITY OF TITANIUM–DIOXIDE, ZIRCONIUM–TIN–TITANATE,
AND ALUMINA IN THE 173–323-K TEMPERATURE RANGE

permittivity. We can also observe in Fig. 2 that the amplitude of

the pulses decreases with the temperature. This decrease may be
attributed to two factors, i.e., the increase of the reflectivity at
the interface due to the increase of the permittivity and a larger
absorption by the sample.
As was described in Section II, we solve (2) numerically to
better quantify the changes on the permittivity and losses in tita-
nium–dioxide. The permittivity is plotted in Fig. 3(a) versus the
frequency for different temperatures, while the loss tangent is
represented in Fig. 3(b). The data presented in these plots range
from 0.2 to 0.8 THz. Above 0.8 THz, the sample is optically
thick and no terahertz radiation was transmitted. Characteristic
error bars are shown at some frequencies of the measurement at
K. The decrease of the permittivity when the tempera-
ture is increased can be clearly seen in Figs. 3(a) and 4(a).
In the range from 173 to 323 K the temperature dependence
of the permittivity of our samples is well described in terms of
a temperature coefficient [18]

(4)

This temperature coefficient defines the relative change of

when the temperature is changed by 1 K. In Fig. 4(a), the mea-
sured values of the permittivity at 500 GHz (circles) are plotted
versus the temperature. The line in this figure is a fit of (4) to the
data from which we obtain the temperature coefficient . The
values of at 300, 500, and 700 GHz are given in Table I.
As can be seen from this table and in Fig. 3(a), a relatively
large decrease of the permittivity of 10 K is obtained
for all frequencies. On the other hand, the loss tangent of tita-
nium–dioxide is nearly constant with temperature. Since in-
creases as the temperature is lowered, this nearly constant value
of implies an increase of and the absorption coefficient.
Titanium–dioxide is a polar material, which means that a sig-
nificant contribution to its permittivity is due to the orientational
molecular polarizability [19], [20]. The average molecular mo-
ment is zero at high temperatures, due to the random orientation
of the molecular dipoles. As the temperature is lowered, these
dipoles align, leading to an increase of the orientational molec-
ular polarizability, which results in a larger permittivity and ab-
sorption.
The very large permittivity of titanium–dioxide makes this
material very appealing for applications in the terahertz regime.
However, its high thermal coefficient of the permittivity makes
it unsuitable for applications in which the temperature cannot
be controlled and a high stability is required. On the other hand,
Fig. 5. (a) Permittivity and (b) loss tangent of the zirconium–tin–titanate
specimen measured at different temperatures. Characteristic error bars are
indicated on the data measured at 10 K (solid gray).
titanium–dioxide is a very good candidate for tunable devices if
the temperature can be controlled [5].
B. Zirconium–Tin–Titanate
The thickness of the considered zirconium–tin–titanate spec-
imen is m. Fig. 5(a) displays the per-
mittivity of zirconium–tin–titanate in a frequency range from
0.2 to 0.7 THz for different temperatures. The loss tangent is
presented in Fig. 5(b). Characteristic error bars are given for
10 K in both plots. As can be appreciated from Fig. 5(a) and
(b), zirconium–tin–titanate has a thermally stable permittivity
and the loss tangent changes only slightly under varying tem-
peratures. The difference between at 173 K and at 323 K is
below 0.25 for all frequencies. Table I displays the values of the
thermal coefficient of the permittivity of zirconium–tin–ti-
tanate for the frequencies 300, 500, and 700 GHz. These coeffi-
cients are obtained by fitting (4) to the measured values of at
different temperatures. These values at 500 GHz and the corre-
sponding fit are plotted in Fig. 4(b) with circles and a solid line,
1270
Fig. 6. (a) Permittivity and (b) loss tangent versus the frequency of alumina
given at different temperatures. Characteristic error bars are indicated on the
data at 10 K (solid gray).
respectively. As can be seen in Table I, is two orders of magni-
tude smaller in zirconium–tin–titanate than in titanium–dioxide.
Zirconium–tin–titanate ceramics are designed to provide high
thermal stability and have turned out to be very popular res-
onator dielectrics in the microwave region [21]. This material
is very promising for applications also in space because it com-
bines a high dielectric constant, low losses, and a low thermal
coefficient of the dielectric constant.
C. Alumina
The alumina specimen has a thickness of
m. Fig. 6(a) displays the permittivity of alumina
in the frequency range from 0.5 to 3.0 THz. The different lines
in Fig. 6(a) correspond to measurements at various tempera-
tures. The values of at different temperatures for a frequency
of 1 THz are given in Fig. 4(c), together with a fit of (4) to
the measurements. In contrast to zirconium–tin–titanate and
titanium–dioxide, the temperature coefficient of the permit-
tivity of alumina is positive in the investigated frequency range.
This means that increases slightly as the temperature is
increased, as can be appreciated in Fig. 4(c). In Table I,
is given for 0.5, 0.7, 1, 2, and 2.75 THz. The loss tangent of
alumina is displayed in Fig. 6(b). As can be seen in this plot,
the loss tangent is comparably low and has a weak dependence
on the temperature. Although alumina has a low permittivity
compared to other high- materials, it is widely used as a
microwave ceramic. This is mainly because of its low price,
good processing properties, and high thermal conductivity [22].
IEEE TRANSACTIONS ON MICROWAVE THEORY AND TECHNIQUES, VOL. 53, NO. 4, APRIL 2005
IV. CONCLUSION
We have studied the change of the complex permittivity with
the temperature of three high- microwave materials, i.e., tita-
nium–dioxide TiO , alumina Al O , and zirconium–tin–ti-
tanate Zr Sn TiO at terahertz frequencies. We have mea-
sured the transmission of broad-band terahertz radiation through
the materials using a terahertz time-domain spectrometer in a
temperature range from 10 to 325 K. Terahertz time-domain
spectroscopy provides data of a far wider frequency spectrum
than earlier methods [23]. All samples show a positive depen-
dence on frequency of both the permittivity and loss parame-
ters, eventually indicating the presence of higher frequency res-
onances or the onset of Rayleigh scattering. Of the three inves-
tigated samples, i.e., the zirconium–tin–titanate ceramic, proves
to be the most suitable for applications under varying environ-
mental conditions because it combines a large real part of the
permittivity ( 37) with low losses and a good thermal stability.
The large permittivity of titanium–dioxide and its strong tem-
perature dependence makes this material suitable for thermally
tunable devices. A possible way to reduce the temperature de-
pendence of the permittivity of high-dielectric constant mate-
rials is by using composite structures such as that of alumina
and titanium–dioxide described in [24].
ACKNOWLEDGMENT
The authors wish to thank C. Janke, S. Sudjana, and F. Spöler,
all with the Institute of Semiconductor Electronics, Rheinisch
Westfaelische Technische Hochschule Aachen (RWTH)
Aachen, Aachen, Germany, for their assistance during the
measurements and many fruitful discussions and D. Schillings
for correcting this paper’s manuscript.
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Klaus Berdel (S’04) was born in Düsseldorf, Ger-
many, in 1978. He is currently working toward the
Dipl.-Ing. in electrical engineering with the Institut
für Halbleitertechnik, Rheinisch Westfaelische Tech-
nische Hochschule (RWTH) Aachen, Aachen, Ger-
many. The main topics of his studies are image pro-
cessing and optoelectronics, embedded systems, and
communication networks.
Since October 2002, he has been a Student Re-
search Assistant with the Institute of Semiconductor
Electronics (IHT), RWTH Aachen. His research in-
terests are terahertz technology, photonic-bandgap structures, and terahertz plas-
monics.
Jaime Gómez Rivas was born in Madrid, Spain,
in August 1971. He received the M.S. degree in
astrophysics from the University Complutense,
Madrid, Spain, in 1995, and the Ph.D. degree in
experimental physics from the University of Am-
sterdam, Amsterdam, The Netherlands, in 2002.
His doctoral dissertation concerned the propagation
of light in strongly scattering semiconductors and
localization of light.
From 1995 to 1996, he was with the Space Re-
search Organization Netherlands (SRON), Utrecht,
The Netherlands, where he investigated the diffusion of quasi-particles in su-
perconducting tunnel junctions for X-ray spectroscopy. In 1997, he joined the
University of Amsterdam. Since August 2002, he has been with the Institute
of Semiconductor Electronics (IHT), Institut für Halbleitertechnik, Rheinisch
Westfaelische Technische Hochschule (RWTH) Aachen, Aachen, Germany.
View publication stats
1271
Peter Haring Bolívar (M’02) was born in Mexico
City, Mexico, in 1969. He received degrees from
the Rheinisch-Westfälische Technische Hochschule
(RWTH) Aachen, Aachen, Germany. During his
thesis, he made the first observation of Bloch oscil-
lations, a fundamental phenomenon predicted since
the beginnings of the 20th Century.
From 1992 to 1993, he was Head of the Rescue
Equipment Division, Nautica Diesel Europea,
Mexico City, Mexico. From 1993 to 1996, he
was a Scientific Assistant with the Institute of
Semiconductor Electronics (IHT), Institut für Halbleitertechnik, Rheinisch
Westfaelische Technische Hochschule (RWTH) Aachen, Aachen, Germany,
where he was involved with conjugated polymers and femtosecond dynamics
in semiconductors. From 1997 to 2001, he was Head of ultrahigh-frequency
research with the IHT, RWTH Aachen, where he directed applied and
fundamental scientific research on coherent terahertz spectroscopy and ultra-
high-frequency optical characterization of electronic gigahertz devices. Since
2001, he has been Head of research at the same institution with ample activities
in the fields of opto-electronics, ultrafast science, ultrahigh-frequency devices,
optical data storage, and nanotechnology. He is currently with the Institute
of High Frequency and Quantum Electronics, University of Siegen, Siegen,
Germany. He has authored or coauthored five book contributions and over 130
publications and international conference presentations. He holds three patents.
Dr. Bolívar was the recipient of a Heinrich Hertz Fellowship presented by
the Science and Research Ministry of the State of Northrhine–Westfalia for his
doctoral research. He was also the recipient of the Wilhelm Borchers Medallion
of the RWTH Aachen.
Peter de Maagt (S’88–M’88–SM’02) was born
in Pauluspolder, The Netherlands, in 1964. He
received the M.Sc. and Ph.D. degrees from the
Eindhoven University of Technology, Eindhoven,
The Netherlands, in 1988 and 1992, respectively,
both in electrical engineering.
He is currently with the European Space
Agency–European Space Research and Technology
Centre (ESA–ESTEC), Noordwijk, The Netherlands.
His research interests are in the area of millimeter-
and submillimeter-wave reflector and planar inte-
grated antennas, quasi-optics, photonic-bandgap antennas, and millimeter- and
submillimeter-wave components.
Dr. de Maagt was the corecipient of the H. A. Wheeler Award presented by the
IEEE Antennas and Propagation Society (IEEE AP-S) for the best applications
paper of 2001. He was also the recipient of a 2002 ESA Award for Innovation.
Heinrich Kurz was born in Austria, in 1943. He re-
ceived the Ph.D. degree from the University of Vi-
enna, Vienna, Austria, in 1971.
From 1971 to 1980, he was Scientific Staff
Member with Philips Research Laboratories, Ham-
burg, Germany, where he was engaged in research
on optical storage and data processing. From 1981
to 1984, he was a Research Associate with Harvard
University, during which time his scientific interest
was directed toward the interaction of ultrashort
laser pulses with semiconductors. Since 1985, he
has been a Professor of electric engineering with the Rheinisch-Westfälische
Technische Hochschule (RWTH) Aachen, Aachen, Germany. His research
includes nonlinear optics, femtosecond laser interactions, and spectroscopy
and application of ultrashort laser pulses in electrical engineering and material
science. Since 1990, he has been the Head of the Institut für Halbleitertechnik,
RWTH Aachen, taking the Chair of Semiconductor Electronics. His main
research activities have been extended to nanoelectronics, mainly silicon-based
nanoelectronics and nanotechnology in general for information science. In
1993, he founded the AMO GmbH, a nonprofit organization, to promote science
and technology from university research into strategic industrial areas. Since
1997, he has been the Scientific Director of the Advanced Microelectronic
Center Aachen (AMICA) built by the AMO GmbH. Since 1998, he coordinates
the national efforts in Germany on nanoelectronics and functional lateral
nanostructures in general.