Integrated Ferroelectrics

ISSN: 1058-4587 (Print) 1607-8489 (Online) Journal homepage: http://www.tandfonline.com/loi/ginf20

Pulsed laser deposition of pyroelectric pclt thin

films using a ceramic/metal target

Lirong Zheng , Pingxiong Yang , W-Ping Xu , Chenglu Lin , Wenbiao Wu &

Masanori Okuyama

To cite this article: Lirong Zheng , Pingxiong Yang , W-Ping Xu , Chenglu Lin , Wenbiao
Wu & Masanori Okuyama (1998) Pulsed laser deposition of pyroelectric pclt thin
films using a ceramic/metal target, Integrated Ferroelectrics, 20:1-4, 73-78, DOI:
10.1080/10584589808238770

To link to this article: http://dx.doi.org/10.1080/10584589808238770

Published online: 27 Sep 2006.

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 Integrared Ferroeleclrics, 1998, Vol. 20, pp. 73-78 0 1998 OPA (Overseas Publishers Associauon) N.V.
Reprints available directly from the publisher Published by license under
Photocopying permitted by license only the Gordon and Breach Science
hblishers imprint.
Printed in India.

PULSED LASER DEPOSITION OF

PYROELECTRIC PCLT THIN FILMS
USING A CERAMIC/METAL TARGET
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LIRONG ZHENG a** , PINGXIONG YANG a,

W-PING XU a , CHENGLU LIN a , WENBIAO WU
and MASANORI OKUYAMA
a State Key Laboratory of Functional Materials for Informatics, Shanghai
Institute of Metallurgy, Chinese Academy of Sciences, Shanghai 200050, China;
Department of Electrical Engineering, Faculty of Engineering Science,
Osaka University, Toyonaka, Osaka 560, Japan

(Received 25 September 1996; In finalform 26 December 1996)

In this paper, we report the preparation and characteristics of Ca and La doped PbTi03
(PCLT) thin film on Pt/Ti/SiO*/Si substrate by laser ablating a ceramic/metal target. The
deposited film is polycrystalline and exhibits good ferroelectric hysteresis loop, low
leakage, and good pyroelectric properties. The pyroelectric coefficient of the film is high
as 8.81 x lo-* C/cm*K and the effective dielectric constant of the film is about 352. So the
figure of merit of the film is high as 0.78~10-'~Ccm/J,indicating that PCLT is a
promising material for pyroelectric application.

Keywords: Pulsed laser deposition; pyroelectric thin film; ceramic/metal target

INTRODUCTION

The pyroelectric infrared (IR) detector has advantages of wavelength

independent sensitivity and room-temperature operation. It has been
expected to provide thermal images for objects at near ambient
temperature."] PbTi03 is an attractive material for the IR detector,

*Corresponding author.

13
 74 L. ZHENG et al.

because it has a large pyroelectric coefficient y and small dielectric

constant E,. The modification of PbTi03 with La or Ca reduces the
tetragonality and the Curie temperature and therefore increases the
pyroelectric coefficient y. Up to now, much attention has been given
to fabrication La doped PbTi03 (PLT) thin films on silicon-based
substrates for monolithic IR detector However, Ca doped
PbTi03 (PCT) gives better pyroelectric performance due to a lower
permittivity and a lower dielectric loss. So far, preparation of Ca
doped lead titanate thin films seems to be very promising for pyro-
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electric applications.
In this paper, we report the deposition of Ca and La doped lead
titanate (PCLT) thin film on Pt-coated silicon by laser ablating a
ceramic/metal target. Well crystallized polycrystalline film was
successfully obtained on Pt/Ti/Si02/Si substrate. The film shows a
large pyroelectric coefficient y of 8.81 x lo-' C/cm2K and a relatively
low dielectric constant E, of 352. Good ferroelectric hysteresis loop is
also obtained in this film.

EXPERIMENTAL

The deposition process was carried out using an ArF pulsed excimer
laser as we described in Ref. [5]. The energy fluency of the laser was
set to 2J/cm2 and the frequency of the pulse was 3Hz. In order to
compensate the loss of Pb content in the film, a ceramic/metal target,
which consists of PCLT ceramic target with composition of 80/10/10
and a lead metal wafer (as shown in Fig. l), is used. So far, the laser
can irradiate partially on the ceramic target and partially on the lead
wafer to provide sufficient Pb content in the film. During deposition,
high pure oxygen was introduced into the chamber and the pressure
of the chamber was maintained at 30Pa. The substrates used in this
experiment were Pt( 1 11)/Ti/Si02/Si (Pt-coated silicon) which was
prepared by electron-beam evaporation in a ultra high vacuum
system at room temperature. The substrate temperature for PCLT
deposition was set to 400-470°C. In order to crystallize the film
into pure perovskite phase, post-annealing of 600°C for 15min
was performed.
 PYROELECTRIC PCLT THIN FILMS 15
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FIGURE 1 Schematic diagram of the ceramic/metal target used for PCLT deposi-
tion.

RESULTS AND DISCUSSIONS

The crystallinity of the film was checked by X-ray diffraction (XRD)

at room temperature. Figure 2 shows the XRD patterns of the film
before and after annealing. We find that 400°C as-deposited film is

15 20 25 30 35 40 45 50 55
2 6 (deg.)
FIGURE 2 XRD patterns for 400°C-deposited PCLT film (a) before and (b) after
annealing, and for 470°C-deposited PCLT film (c) before and (d) after annealing.
 16 L. ZHENG ef al.

microcrystalline and has a main diffraction peak near 29.7”, which

corresponds to the (222) peak of pyroelectric phase as marked by
“Py.” in Figure 2(a). After 600°C annealing for 15 min, the film has
been completely transferred into pure perovskite phase and it has a
main diffraction peak of (1 10) [Fig. 2(b)]. The 470°C as-deposited film
is almost perovslute phase, and has a main diffraction peak of (100)
[as shown in Fig. 2(c)]. After annealing, the trace of pyrochlore has been
completely removed, and the film is highly (100) oriented. The result
indicates that the crystal orientation of the film is mainly dependent on
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the substrate temperature. However, we find that it is difficult to

develop a c-axis orientation of the film on such kind substrates.
Figure 3 shows the ferroelectric hysteresis loop of the film measured
by a modified Sawyer-Tower circuit at 50 Hz. The film was deposited
at 400°C followed by 600°C annealing for 15min and its thickness is
about 0.4pm. The remanent polarization of the film is found to be
about 13.6 pmC/cm2 and the coercive field is about 40 KV/cm,
indicating good ferroelectric property of the film. The dielectric
constant of this film was measured by a I KHz C-V plot. It was found
that the effective dielectric constant of the film E, was about 352 at zero
biased field, which is smaller than that of polycrystalline PLT(80/10)
and PLT(85/15).L61While at coercive field, it can reach to 965 due to
the polarization reversal. The dielectric loss of the film is found to be
less than 0.02 when the test frequency is less than 1 MHz.

X: 2Vldiv t
I I I

FIGURE 3 A typical P-E hysteresis loop of the PCLT thin film.

 PYROELECTRIC PCLT THIN FILMS I1

Leakage current of the film plotted as a function of applied voltage

is shown in Figure 4. The leakage current density is about lop7 A/cm2
under 3 V bias, which corresponds a resistivity of about 7 . 5 10"~ Ocm.
The pyroelectric coefficient y were determined from the change of
spontaneous polarization P, of the sample at different temperatures T,
i.e., y = dP,/dT. Figure 5 shows an almost linear decrease of P, when
the temperature of film increases from 0°C to 100°C. The sample in
this figure was deposited at 400°C then followed by 600°C annealing
for 15 min and its thickness is about 0.4 pm. From the figure we obtain
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a high y of about 8.81 x C/cm2K for this sample. The figure of

merit Fv(= y/(&,C,): where C, is volume-specific heat) of this sample is
about 0 . 7 8 ~10-'°Ccm/J, which is larger than that of PLT(90/10) film
on Pt/MgO reported by Iijima et (where the c-axis orientation ratio
of the film is 0.75 and F, M 0 . 5 3 lO-'OCcm/J)
~ and is very close to their
c-axis oriented PbTi03 film on Pt/MgO (F, = 0.8 x lo-'' C C ~ / J ) . [ ~ I

CONCLUSIONS

We have successfully prepared PCLT thin film on Pt-coated silicon

substrate by laser ablating a ceramic/metal target. Though the deposi-
ted films are polycrystalline and seem difficult to be c-axis oriented on

Applied Voltage (v)

FIGURE 4 Leakage-voltage characteristic of the PCLT thin film.
 78 L.ZHENG et al.

y = 8.81X 10-8 C/cm2K

40 -

3 0 , ~
0
a2 20-
a"
10 -
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- 4B' PCLT(80/1O/lO)
I I
0- I 1

FIGURE 5 Dependence of the spontaneous polarization of the film on the sample's

temperature.

Pt-coated silicon, they exhibit a high pyroelectric coefficient and a

relatively low dielectric constant due to Ca doping and hence a high
figure of merit. The deposited films also exhibit good ferroelectric
property and high resistivity. The experimental result indicates that Ca
doped PbTi03 film is a promising material for pyroelectric IR detector
arrays.

References

[l] Okuyarna, M. and Hamakawa, Y . (1991). Ferroelectrics, 118, 261.

[2] Peterson, G. A,, Zou, L. C. and Van Buren, W. M. (1990). Mut. Res. Soc. Proc., 200,
127.
[3] Patel, A,, Tossell, D. A., Shorrocks, N. M., Whatmore, R. W. and Watton, R. W.
(1993). Mat. Res. SOC.Proc., 310, 53.
[4] Iijima, K., Takayama, R., Tomita, Y . and Ueda, I. (1986). J. Appl. Phys., 60(8),
2914.
[5] Zheng, L., Zhang, S. and Lin, C . (1996). Acta Phys. Sinica., 5(5), 384.
[6] Lee, S. S. and Kim, H. G., 3rd Pacific Rim Con$ on Ferroelectric Applications,
Kyoto Japan, May 1996.
[7] Iijima, K., Takayama, R., Tomita, Y. and Ueda, I. (1986). J . Appl. Phys., 68(8),
2914.