Flexible piezoelectric pressure sensors using oriented aluminum nitride thin films

prepared on polyethylene terephthalate films

Morito Akiyama, Yukari Morofuji, Toshihiro Kamohara, Keiko Nishikubo, Masayoshi Tsubai, Osamu Fukuda, and
Naohiro Ueno

Citation: Journal of Applied Physics 100, 114318 (2006); doi: 10.1063/1.2401312

View online: https://doi.org/10.1063/1.2401312
View Table of Contents: http://aip.scitation.org/toc/jap/100/11
Published by the American Institute of Physics

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 JOURNAL OF APPLIED PHYSICS 100, 114318 共2006兲

Flexible piezoelectric pressure sensors using oriented aluminum nitride

thin films prepared on polyethylene terephthalate films
Morito Akiyama,a兲 Yukari Morofuji, Toshihiro Kamohara, Keiko Nishikubo,
Masayoshi Tsubai, Osamu Fukuda, and Naohiro Ueno
On-site Sensing and Diagnosis Research Laboratory, National Institute of Advanced Industrial Science and
Technology, 807-1 Shuku, Tosu, Saga 841-0052, Japan
共Received 13 July 2006; accepted 8 October 2006; published online 12 December 2006兲
We have investigated the high sensitive piezoelectric response of c-axis oriented aluminum nitride
共AlN兲 thin films prepared on polyethylene terephthalate 共PET兲 films. The AlN films were deposited
using a radio frequency magnetron sputtering method at temperatures close to room temperature.
The c axes of the AlN films were perpendicularly oriented to the PET film surfaces. The sensor
consisting of the AlN and PET films is flexible like PET films and the electrical charge is linearly
proportional to the stress within a wide range from 0 to 8.5 MPa. The sensor can respond to the
frequencies from 0.3 to over 100 Hz and measures a clear human pulse wave form by holding the
sensor between thumb and middle finger. The resolution of the pulse wave form is comparable to a
sphygmomanometer at stress levels of 10 kPa. We think that the origin of the high performance of
the sensor is the deflection effect, the thin thickness and high elastic modulus of the AlN layer, and
the thin thickness and low elastic modulus of the PET film. © 2006 American Institute of Physics.
关DOI: 10.1063/1.2401312兴

I. INTRODUCTION be synthesized using several techniques, such as reactive

sputtering,15,16 molecular beam epitaxy, laser ablation, and
Human pulse wave form analysis is an important tech-
chemical vapor deposition.17–19 Among these methods, the
nology for screening subjects for early evidence of a variety
reactive sputtering technique is considered to be the favor-
of vascular diseases and cardiovascular disorders and in
able selection because of its easily deposited high 共0001兲
monitoring the response to therapy.1–4 Various pulse wave
orientation at relatively low temperature and compatibility
sensors have already been developed; a photoelectric method
with standard integrated circuit 共IC兲 technology. Moreover,
with an infrared light-emitting diode and a semiconductor
AlN is a high temperature piezoelectric material, and it is
pressure sensor with an arm compression cuff are usually
estimated that AlN keeps piezoelectric characteristics at tem-
used.2–7 However, these pulse wave sensors are not suitable
perature up to 1150 ° C.10,20,21 AlN does not require a subse-
for measuring a complex pulse wave form compared to an
quent electric-thermal poling such as ferroelectrics, and it is
invasive method, and the measuring point of them is
a lead-free piezoelectric ceramic and environment friendly
restricted.4 Various piezoelectric thin films consisting of
material. Polyethylene terephthalate 共PET兲 is polyester, hav-
polymers or ceramics have been widely used in physical
ing a high melting point and very good mechanical strength
sensors.8,9 However, materials with many superior properties
due to the presence of aromatic ring in the polymeric struc-
must be developed, because the demand for change in sensor
ture. It is resistant to heat and moisture and virtually unat-
design exceeds the capabilities of existing materials. We
tached by many chemicals.22,23
have investigated various metals, ceramics, and polymers to
In this work, we describe the crystal state and piezoelec-
develop sensor materials using the characteristics of the three
tric responses of AlN thin films prepared on PET films, ca-
materials. In this study, we have suggested a laminate struc-
pable of measuring a clear complex pulse wave form. Our
ture sensor consisting of metal electrodes, a piezoelectric ce-
sensor, composed of platinum 共Pt兲 thin films, an AlN thin
ramic layer, and a polymer film to develop a piezoelectric
film, and a PET film, directly converts local stress into elec-
material with high sensitivity, high thermal stability, and
tric charge. The high sensitivity is due to the thin-film struc-
flexibility, shown in Fig. 1共a兲.
ture and flexibility.
Aluminum nitride 共AlN兲 is one of piezoelectric ceramic
materials and has high thermal and chemical stabilities. AlN
does not contain any pollution-contribution elements and is a II. EXPERIMENT
hard material 共hardness of 23.7 GPa兲.10,11 Hence, AlN is an AlN thin films were prepared on PET films 共Du Pont-
excellent piezoelectric material. AlN piezoelectric films have Toray兲 by using radio frequency 共rf兲 magnetron reactive
played an increasing role in micro- and nanoelectromechani- sputtering system 共Tokuda CFS-4ES兲.24 A commercial 3 in.
cal systems 共MEMS, and NEMS兲 and in bulk acoustic wave diameter Al metal 共99.999% pure兲 was used as a target. The
共BAW兲 devices for resonators and filters in high-frequency distance between the PET films and the target was about
communication components.12–14 Generally, AlN films can 8.3 cm. The sputtering chamber was evacuated to below 5
⫻ 10−4 Pa, and sputtering atmosphere was mixed Ar
a兲
Electronic mail: m.akiyama@aist.go.jp 共99.999% pure兲 and N2 共99.999% pure兲 gases at 0.3 Pa. Be-

0021-8979/2006/100共11兲/114318/5/$23.00 100, 114318-1 © 2006 American Institute of Physics

114318-2 Akiyama et al.
fore the deposition process, the Al target was precleaned at
the same deposition conditions for about 5 min with the
shutter closed. The radio frequency power was kept at
400 W. Deposition was carried out at room temperature 共no
heating兲. Pt electrodes were deposited with the same sputter-
ing system. A commercial 3 in. diameter Pt metal target
共99.9%兲 was used for the deposition. Only argon was used as
the working gas 共0.5 Pa兲 and the power was kept at 200 W.
The deposition was carried out at room temperature. The
samples were observed using a field-emission scanning elec-
tron microscope 共FE-SEM兲 共Hitachi S-4300兲. The crystal
structure and crystallinity of the AlN films were measured
with x-ray diffraction 共Philips X’Pert兲 analysis using Cu K␣
radiation, and the crystal orientation was evaluated using the
full width at half maximum 共FWHM兲 of the x-ray rocking
curves of the 共0002兲 diffraction peaks of the AlN films.
III. RESULTS AND DISCUSSION
We have suggested the laminate sensor structure, shown
in Fig. 1共a兲. The sensor consists of Pt 共0.1 ␮m thick兲, AlN
共1 ␮m thick兲 layer, and PET 共9 ␮m thick兲 film to obtain
sensitivity, flexibility, and fatigue durability. The Pt elec-
trodes are separated by the PET film, because the PET film
plays important roles as a flexible substrate and an insulating
layer to avoid unexpected leakage of electric charges. The
AlN layer is smooth, transparent, and electrically insulating.
Figure 1共b兲 shows the FE-SEM image of the cross sectional
of the AlN layer. The SEM image indicates that the AlN
layer consists of innumerable oriented columnar fine grains,
which are perpendicular to the PET film surface. The grain
diameter is around 80 nm. This result means that AlN colum-
nar nanograins can grow on a PET film. Figures 1共c兲 and
1共d兲 show the x-ray diffraction 共XRD兲 pattern and x-ray
J. Appl. Phys. 100, 114318 共2006兲
FIG. 1. 共Color online兲 Multilayer
structure of flexible pressure sensor.
共a兲 Schematic diagram of sensor struc-
ture showing Pt electrodes, AlN, and
PET films. 共b兲 Typical FE-SEM image
of cross-sectional structure of AlN
film deposited on PET film. 共c兲 X-ray
diffraction pattern of AlN film depos-
ited on PET film. Cu K␣ radiation was
used. 共d兲 X-ray rocking curve of AlN
film.
rocking curve of the AlN, respectively. Only one peak at
36.04° is observed except for the peaks of the PET film and
the Pt electrodes. The peak intensity is quite low, and the
peak position consists with the 共0002兲 diffraction peak of
hexagonal AlN. From this result, we think that the crystal
structure of the AlN film is hexagonal AlN, and the nan-
ograin c axis orients perpendicular to the PET film surface.
The FWHM of the x-ray rocking curve was 11.7°, which is
larger than that of AlN thin films deposited on amorphous
and single crystal substrates,25–28 indicating that the crystal
orientation is comparatively low. Shiosaki et al. used PET
sheets 共72 ␮m thick兲 as substrates for AlN films to fabricate
a piezoelectric speaker. However, they did not directly pre-
pared AlN films on PET sheets and deposited aluminum
films as bottom electrodes on PET sheet surfaces.29 Hence,
there is no report that AlN films are directly prepared on PET
films. We have prepared c-axis oriented AlN thin films on a
PET film by rf reactive sputtering without heating.
We investigated the piezoelectric responses of the sensor
consisting of the Pt electrodes, AlN, and PET films in a pres-
sure range from 0 to 8.5 MPa with a vibration exciter at
room temperature, shown in Fig. 2共a兲. The pressure-induced
electric charge of the sensor is consistent with the load cell
signal. Figure 2共b兲 shows the dependence of the electric
charge on pressure. The electrical charge is linearly propor-
tional to pressure for the range. The piezoelectric response
共the induced charge per unit force applied in the same direc-
tion兲 of the sensor was 0.7 pC/ N. The reported piezoelectric
coefficient d33 of single crystal AlN thin films is
3 – 5 pC/ N,30–33 and the piezoelectric response of the sensor
is comparatively low. Furthermore, we measured the piezo-
electric response of the same device without AlN layer, and
the device did not response to pressure. We think that the low
piezoelectric response is due to the low crystallinity and
114318-3 Akiyama et al. J. Appl. Phys. 100, 114318 共2006兲

FIG. 2. 共Color online兲 Characteristics of piezoelectric pressure sensor. 共a兲

Schematic of setup to evaluate piezoelectric response of sensor. The electric
charge from the AlN film is measured with a charge amplifier and an oscil-
loscope. 共b兲 Relationship between pressure and electric charge of sensor.
The frequency is 10 Hz. 共c兲 Dependence of gain and phase of sensor on
frequency. The load and offset are 20 and 40 N.

crystal orientation of the AlN film, shown in Figs. 1共c兲 and

1共d兲.33,34 Figure 2共c兲 shows the dependence of the sensor
response on frequency. Gain is attenuation ratio and is de-
fined as 20 log10共x / y兲 共dB兲 in this study, where x is a mea-
sured value, and y is a reference value which is measured at
1 Hz. The gain is constant from 0.5 to 100 Hz, and de-
creases below 0.4 Hz. It is thought that the gain is decreased
by the leak of the generated charges, because the electric
resistance of the sensor is not infinity.35 On the other hand,
the phase is constant over 4 Hz, and increases below 3 Hz.
The limit of our measurement equipment was 100 Hz, and
we estimate that the sensor can response to higher frequency
than 100 Hz, because AlN is a hard material 共hardness
27 GPa兲.10,11
To evaluate the capabilities of the sensor for measuring
human pulse wave forms, we compared the sensor with a
commercial sphygmomanometer. Figure 3共a兲 shows the
schematic diagram of the sensor structure. The sensor con-
sists of the fold multilayered film. The internal Pt electrode is
shielded by the external Pt electrode, because the structure
contributes to avoiding unexpected noise. Furthermore, the
two AlN layers generate double the amount of electric charge
in comparison with the single layer one. It is well known that
the voltage V produced by a piezoelectric is calculated using
the following expression:36 V = Fg33d / A, where F is the
force, g33 is the voltage output coefficient, d is the thickness
of the piezoelectric, and A is the surface area of the piezo-
electric. The electric charge is calculated as follows: Q
= CV, where Q is the electric charge and C is the capaci-
FIG. 3. 共Color online兲 Comparison of pressure sensor and electric sphyg-
momanometer. 共a兲 Schematic diagram of sensor structure. 共b兲 Photograph of
actual test setup to measure pulse wave forms with sensor and sphygmoma-
nometer. 共c兲 Human pulse waves measured with sensor and
sphygmomanometer.
tance; C = ␧A / d, where ␧ is the permittivity; and Q = ␧AV / d
= ␧g33F = ␧g33AP, where P is the pressure. This reveals that
the sensitivity of the sensor to pressure is proportional to the
surface area. The pulse wave sensor has the characteristic
that the larger the surface area of the sensor, the higher the
sensitivity of the sensor. The characteristic differs from that
of general pressure sensors. We measured our pulse waves
by using the sensor. The sensor was fixed by our thumb and
middle finger to measure pulse wave forms at our finger tips,
shown in Fig. 3共b兲. The pulse waves were simultaneously
measured at wrist with a sphygmomanometer to evaluate the
sensor response. Figure 3共c兲 shows the typical pulse wave
forms of the sensor and sphygmomanometer. The sensor sen-
sitively responds to pulse waves and definitely detects some
114318-4 Akiyama et al.
waves, such as tidal and preejection waves, which are impor-
tant waves for pulse-wave form analysis or pulse
diagnosis.1–4 The pulse wave forms are clear and show some
fine waves compared to that measured by photoplethysmo-
graphic 共PPG兲 measurements.4,37 The blood pressure is gen-
erally from 85 to 130 mmHg 共10– 17 kPa兲. Hence, the reso-
lution of the pulse wave form is comparable to an electric
sphygmomanometer at stress levels of 10 kPa, although the
sensor is fixed at the finger tip, which is not better than wrist
for measuring pulse wave forms.
To find the origin of the high performance of the sensor,
we investigated the influence of the deflection effect in dia-
phragm structure on the piezoelectric response.38 The sensor
was fixed on a glass cylinder to construct the diaphragm
structure, shown in Fig. 4共a兲. When the pressure is rapidly
decreased to zero by draining nitrogen gas in the air cham-
ber, the electric charge rapidly increases to a maximum value
and gradually decreases after the pressure becomes zero. Fig-
ure 4共b兲 shows the dependence of the electric charge on pres-
sure. The maximum value increases with increasing pressure
and shows an excellent linearity in the range from
0.9 to 400 kPa. The piezoelectric response is found to be
30.0 pC/ N, although the piezoelectric response of the sensor
is 0.7 pC/ N as previously mentioned. These results indicate
that the piezoelectric response of the sensor drastically im-
proves by using the deflection effect. Furthermore, it is re-
ported that the response of a piezoelectric thin film increases
exponentially with decreasing the thickness and elastic
modulus of substrate.38 Therefore, we think that the origin of
the high performance of the sensor is the deflection effect,
the thin thickness and high elastic modulus of the AlN layer,
and the thin thickness and low elastic modulus of the PET
film. Moreover, the sensor is expected as artificial skin for
humanoid robots, because the sensor sensitivity is ⬃0.9 kPa,
which is well within the 10– 40 kPa range that a human fin-
ger applies to sense texture and shape.39
IV. CONCLUSIONS
We have prepared flexible pressure sensors consisting of
Pt electrodes, c-axis oriented AlN thin films, and PET films.
The electrical charge of the sensor is linearly proportional to
J. Appl. Phys. 100, 114318 共2006兲
FIG. 4. 共Color online兲 Influence of diaphragm structure
on piezoelectric response. 共a兲 Top and cross-sectional
view of sensor device, and schematic drawing of setup
to measure piezoelectric response of sensor. The diam-
eters of the PET film and top electrode are 9 and 2 mm,
respectively. 共b兲 Dependence of piezoelectric response
of sensor on pressure.
pressure for the range from 0 to 8.5 MPa. The piezoelectric
response of the sensor was 0.7 pC/ N. The sensor can re-
spond to the frequencies from 0.3 to over 100 Hz and mea-
sures a clear human pulse wave form by holding the sensor
between the thumb and middle finger. We think that the ori-
gin of the high performance of the sensor is the deflection
effect, the thin thickness and high elastic modulus of the AlN
thin film, and the thin thickness and low elastic modulus of
the PET film. The sensor makes full use of the characteristics
of the materials and this study suggests a concept for design-
ing sensor devices.
ACKNOWLEDGMENTS
The authors would like to thank Dr. Kazushi Kishi and
Yasunobu Ooishi of AIST for measuring the piezoelectric
response of the sensor.
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