Preparation of SrTiO3 thin films on Si(100) substrates by laser ablation:

Application as buffer layer for YBa2Cu3O7 films

F. Sánchez, M. Varela, X. Queralt, R. Aguiar, and J. L. Morenza

Citation: Appl. Phys. Lett. 61, 2228 (1992);

View online: https://doi.org/10.1063/1.108276
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Published by the American Institute of Physics

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Preparation of SrTQ thin films on Si(lQ0) substrates by laser ablation:
Application as buffer layer for YBa@& films
F. Stinchez, M. Varela, X. Queralt, R. Aguiar, and J. L. Morenza
Universitat de Barcelona, Departament de Jisica Aplicada i Electrhica, Avenida Diagonal 647,
E-08028 Barcelona, Spain
(Received 28 January 1992; accepted for publication 24 August 1992)
SrTiO, thin films have been deposited on Si( 100) by pulsed laser ablation. The films were
characterized by x-ray diffractometry, field emission scanning electron microscopy, and
secondary ion mass spectrometry. The films show the (hO0) or (hh0) preferential orientations
depending on the substrate temperature and oxygen partial pressure during the deposition.
Depth profiles indicate that films grow without an important reaction with the substrate.
Superconducting YBa&!u,O,-x thin tllms were successfully deposited by laser ablation on
Si( 100) substrates coated with SrTiOs buffer layer. This indicates that SrTiO, is a good material
as a buffer layer for deposition of YBa,Cu307-x on silicon.

The structural and electrical properties of strontium methanol and then etched in a 10% HF solution. After
titanate, STO, are suitable for several applications. Because that, they were introduced in a vacuum chamber, and pre-
of the similar crystalline lattice constants, thermal expan- viously to the deposition, were maintained in vacuum
sion coefficients and its low chemical reactivity, ST0 single ( 1O-8-1O-7 mbar) at a temperature of 850 “C for more
crystals are the most used substrates for growing than 30 min.
YBa&!usO,-, (YBCO) thin films.’ Furthermore, ST0 ST0 thin films were deposited onto the Si substrates by
electrical properties are interesting for numerous electronic laser ablation using an ArF excimer laser ( 193 nm wave-
applications in very large scale integrated (VLSI) circuits length, 23 ns pulse duration) with a repetition rate of 5 Hz.
such as dynamic random access memories (DRAMS ) ’ and The laser beam was led to the vacuum chamber through a
antireflective coatings in optoelectronic devices. In addi- quartz window and was focused at a fluency of about 5
tion, ST0 iilms could be used as very fast oxygen sensors J/cm2 on a stoichiometric target of SrTiO, at an angle of
since their electrical conductivity changes fast with the am- 45”. The substrate was placed parallel to the target at a
bient oxygen partial pressure.3 distance of about 8 cm. The base pressure was around
ST0 has a cubic perovskite structure with a lattice 10-‘-10P7 mbar. During the deposition process high pu-
constant of a s-ro=0.3905 nm, which facilitates the epitax- rity oxygen was introduced and the pressure was fixed in
ial growth of ST0 thin films on Si( 100) substrates. When the 10-5-10-3 mbar range. To prevent oxide regrowth
the ST0 unit cell is rotated 45” around the surface normal during the early stages of the growth process, all deposi-
[loo] axis a mismatch of only 1.7% is observed, whereas a tions were initiated at the base pressure of the vacuum
6.3% is found in the 3asro112asirelation, then it could be system and the oxygen pressure was raised after the first
expected that ST0 grown on Si( 100) will be especially 100 pulses. Films of about 50 nm thick were deposited at a
oriented in the directions (/ZOO) and (hh0). Both ST0 substrate temperature in the 400-750 “C range and at a
crystalline orientations are highly suitable to YBCO epi- deposition rate around 0.035 nm s-l. Afterwards, an
taxial growth and are the common orientations when a YBCO thin film was deposited by laser ablation on ST0
ST0 single crystal is used as substrate. In addition, ST0 coated Si( 100). The main deposition conditions of the
has an intermediate thermal expansion coeficient ( ~8 YBCO films were: 10 Hz of repetition rate, 4 cm of target-
x 10m6 K-‘) between that of YBCO (Z 13 X 10e6 K-l) substrate distance, 0.3 mbar of oxygen pressure and 750 “C
and that of Si ( ~3 X 10M6 K-l). Strontium titanate thin of substrate temperature. The film thickness was 1 ,um and
films have been prepared by rf sputtering,3 electron gun the deposition rate was about 0.45 nm s- ‘.
evaporation4 laser ablation,’ and organometallic chemical The field emission microscopy micrographs of ST0
vapor deposition (OMCVD) .6 Most of these methods need films (Fig. 1) show a very smooth surface without micro-
high deposition temperature and/or post-annealing at high cracks and practically free of particles. This morphology is
temperature. Laser ablation seems to be the best technique quite different to that reported for films obtained by other
to obtain epitaxial as-deposited films at relatively low tem- methods which show a very granular structure.6 This is
peratures and ST0 has been already used as a buffer layer noteworthy because the growth of YBCO superconducting
on silicon and on sapphire.’ However, a complete study of films on ST0 coated silicon requires a clean and smooth
the deposition of ST0 on Si by laser ablation, has not been surface.
realized yet, and in this work we present the studies of the Figure 2 shows the x-ray diffraction (XRD) spectrum
ST0 film properties dependence with the technological pa- of ST0 film deposited at a oxygen partial pressure of lo-’
rameters. mbar and a substrate temperature of 750 “C!. The films
The Si( 100) substrates were prepared to remove the have, in all the cases, only the STO’s peaks with preferen-
native oxide. For this purpose, Si( 100) wafers were tial orientation (hO0) or (hh0). The intensity relation be-
cleaned ultrasonically with trichloroethylene, acetone, and tween (200) and ( 110) peaks as a function of pressure and

2228 Appl. Phys. Lett. 61 (la), 2 November 1992 0003~6951/92/432228-03$03.00 @ 1992 American Institute of Physics 2228
 ia)
1.25
i

LO-0 10 -5 10 -.+ 10.-a 10-e

Pressure (mbar)

FIG. 1. Field emission micrograph of the surface of a ST0 sample.

temperature is plotted in Fig. 3. In Fig. 3(a) we see, for a

fixed temperature, that the ratio I12&I~,,,, rises as the
oxygen pressure is increased. In Fig. 3 (b) we see, for dif-
ferent pressures, that 1~200~/1~110~ also rises with the tem-
perature, then it seems that it is easy to grow films very
preferentially oriented along the (hO0) direction. It is also
observed that we could have a predominance of the orien-
tation (hhO), although it is limited by the pressure and the
temperature. The pressure dependence is very weak below
lo-” mbar and the deposition at temperature lower than
650 “C! produces a limited crystallinity.
The depth composition profiles of the ST0 films have
been obtained by secondary ion mass specti-ometry ’ 7
-----‘; 750 10
(SIMS). They show good uniformity of Sr, Ti, and 0 in Temperature (“C)
the film, without Si diffusion (Fig. 4). A Sr diffusion is
observed towards Si, though this is not very important
FIG. 3. 1~200~/I~L10~ ratio for ST0 films as’s function of: (a) pressure,
since the Sr signal is uniform in the film. These results are being the substrate temperature 650°C (0 ) and 750°C (0); (b) sub-
in agreement with the absolute absence of strange phases in strate temperature, being the pressure 10e5 mbar (0 ), 10e4 mbar (O),
the XRD spectra. 5X10-’ mbar (A) and 10e3 mbar (0). The dashed line shows the
Figure 5 shows the XRD spectrum of a YBCO film I~zM)~/I~llo~ratio corresponding to a powder sample.
deposited on silicon with a ST0 buffer layer. Although the
highest intensity corresponds to the (103) peak, the YBCO

10 20 30 40 JO 00

P Sputter time (min)

61

FIG. 4. SIMS profile of a ST0 film deposited at a substrate temperature

FIG. 2. XRD spectrum of a ST0 film. of 750 “C.

2229 Appl. Phys. Lett., Vol. 61, No. 18, 2 November 1992 Sanchez et al. 2229
 - -7 ,.a ---- -

l.0

s 0.8
3 2
B z 0.6
G- 2
;; 8
iTf 04
zi
sz 0.2
c E z
‘I 08 z 0 0’
0 0.0
..-4 II 100 150 200

10 20 3’ -20 50 60 70 EOG .O( Temperature (K)

2@ (“)
FIG. 6. Normalized resistance vs temperature for a YBCO film on
FIG. 5. XRD spectrum of a YBCO film deposited on Si( 100) with a ST0 Si( 100) with a ST0 buffer layer.
buffer layer.
The authors would like to thank Dr. R. Fontarnau for
the field electron microscopy micrographs. The authors
film is partially (OOh) textured. The normalized resistance- acknowledge the collaboration of the Secondary Ion Mass
temperature curve of this film is presented in Fig. 6. Zero Spectrometry, and Scientific and Technical Services of
resistance is observed at a temperature of 84.5 K with Universitat de Barcelona. This work is a part of a research
onset temperature at 90.5 K. The width of the supercon- project financed by CICYT of the Spanish Government
ducting transition (lo%-90%) is 4 K. (Project MAT 89-0253) and Red Electrica de EspaEa, S.
In summary, we have shown that laser ablation is an A. (MIDAS Programme).
excellent method for the deposition of ST0 thin films on ‘X. D. Wu, D. Dijkkamp, S. B. Ogale, A. Inam, E; W. Chase, P. F.
Si( 100). The films are very smooth and the reactivity with Mice%, C. C. Chang, J. M. Tarascon, and T. Venkatesan, Appl. Phys.
the substrate is minimum, as revealed by SIMS and XRD. L&t. 51, 861 (1987).
‘T. Sakuma, S. Yamamichi, S. Matsubara, H. Yamaguchi, and Y. Mi-
By adjusting substrate temperature and oxygen partial yasaka, Appl. Phys. Lett. 57, 2431 (1990).
pressure during deposition it is possible to control the rel- 3J. Gerblinger and H. Meixner, J. Appl. Phys. 67, 7453 (1990).
ative intensity between the two crystalline orientations, ‘H. Mori and H. Ishiwara, Jpn. J. Appl. Phys. 30, L1415 (1991).
‘E. Wiener-Avnear, G. L. Kerber, J. E. McFall, J. W. Spargo, and A. G.
(&IO) and (hh0). Finally, we have successfully deposited
Toth, Appl. Phys. Lett. 56, 1802 (1990).
YBCO superconducting thin films on Si( 100) substrates 6W. A. Feil, B. W. Wessels, L. M. Tonge, and T. J. Marks, J. Appl. Phys.
with ST0 buffer layers. 67, 3858 (1990).

2230 Appl. Phys. Lett., Vol. 61, No. 18, 2 November 1992 Sanchez et al. 2230