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Deposition of AlN films by reactive sputtering: Effect of radiofrequency

substrate bias

Article  in  Thin Solid Films · June 2007

DOI: 10.1016/j.tsf.2007.03.006

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 Thin Solid Films 515 (2007) 7105 – 7108
www.elsevier.com/locate/tsf

Deposition of AlN films by reactive sputtering: Effect of radio

frequency substrate bias
B. Abdallah a,d , A. Chala c , P.-Y. Jouan b , M.P. Besland a,⁎, M.A. Djouadi a
a
Institut des Matériaux Jean Rouxel IMN UMR 6502, Université de Nantes, 2 rue de La Houssinière BP 32229, 44322 Nantes Cedex France
b
IUT MPh, Université de Valenciennes et du Hainaut-Cambrésis, Zone Industrielle du Champ de l’Abbesse, 59600 Maubeuge, France
c
Département de Physique, Université de Biskra, BP 145 RP, 07000 Biskra, Algeria
d
Atomic Energy Commission Syrian (AECS), BP 6091, Damascus, Syrian Arab Republic
Received 15 November 2006; received in revised form 6 March 2007; accepted 6 March 2007
Available online 12 March 2007

Abstract

Piezoelectric AlN thin films were deposited on Silicon substrates by triode reactive sputtering. The variation of residual stress versus bias
voltage on the substrate was investigated. A compressive stress was always observed with a maximum value for a negative substrate bias of 50 V.
For higher negative bias voltage values, the compressive stress decreases. X-ray diffraction measurements showed two kinds of growth
orientation. First, without bias voltage, films are well crystallized and (002) oriented. Second, with bias voltage, the (002) orientation disappears
and a small peak appears (situated in the 2θ = 32°–33° range) which can be attributed to (100) orientation. Finally, the influence of compressive
stress and ion bombardment on the change of orientation is discussed.
© 2007 Elsevier B.V. All rights reserved.

Keywords: Aluminium nitride; X-ray diffraction; stress measurements; substrate bias effect

1. Introduction Nevertheless, the very high residual stress observed in AlN

For the last decades, aluminium nitride (AlN) is one of the
more promising piezoelectric material for a wide range of
applications such as optics [1], mechanics and electronics [2,3].
Especially for the later domain, aluminium nitride can exhibit
either a III–V semiconductor or a dielectric behavior [4]. In
addition, since AlN is a piezoelectric material with a high
acoustic velocity [5] and a low density (3.3 g/cm3), it is a good
candidate for high frequency devices, like surface acoustic
waves devices (SAW), resonators, high frequency filters and
pressure sensors working in aggressive environment [6–8].
Moreover, the elaboration of SAW devices on ultra hard
substrates such as diamond-like carbon [9] or c-BN may
increase significantly the work frequency and makes possible to
work in the GHz range.
⁎ Corresponding author.
E-mail address: Marie-Paule.besland@cnrs-imn.fr (M.P. Besland).
0040-6090/$ - see front matter © 2007 Elsevier B.V. All rights reserved.
doi:10.1016/j.tsf.2007.03.006
films results in deterioration of the performances of SAW
devices as well as shorter lifetimes.
In this work the stress evolution in AlN films was studied as
a function of negative bias voltage and related to the structure of
the films. Attempts were made in order to understand the effect
of high bias on the orientation of aluminium nitride thin films.
2. Experimental details
The triode sputtering system used in this work has been
described previously [10]. Briefly, a plasma discharge was
created by an emitting tungsten filament and a planar anode. A
residual pressure in the 10− 4-Pa range was achieved using a
diffusion pump and working pressure was ranging from 0.05 to
0.5 Pa. High ionization rate was obtained thanks to magnetic
coils. Depositions of AlN films were carried out with a 100-mm
diameter target of pure aluminium (99.98%), direct current
(DC) biased, in Ar/N2 reactive discharges. The Cu substrate
holder, located at 40 mm from the substrate, was negatively
biased with a radiofrequency (RF) voltage varying in the 0- to
7106 B. Abdallah et al. / Thin Solid Films 515 (2007) 7105–7108
250-V range. The spontaneous heating by the DC plasma gave a
substrate temperature between 400 K and 500 K depending on
the substrate bias. (100) oriented silicon wafers were used as
substrates. The self bias voltage Vb is given by RF generator. If
we assume that the sheath in front of the substrate is lower than
the mean free path of the particles (neutrals, ions and
molecules), it is easy to deduce the energy of ions impinging
the substrate during deposition process : E = e(Vp − Vb) where
Vp is the plasma potential of the discharge [10]. Then the energy
of ions varies between 30 eV and 280 eV.
Before each deposition, the aluminium target was cleaned in
an argon discharge lasting 20 min and pre-sputtered for 20 min
as well. A shutter in front of the target prevents deposition on
substrates during these periods. In the present work, the
deposition parameters, gathered in Table 1, were as follows:
filament current 20 A, target voltage − 1000 V, target current
100 mA, coil current 3 A, anode voltage + 150 V. Stoichiometric
AlN films were obtained at a working pressure of 0.3 Pa (10%
N2–90% Ar).
Film thickness and substrate curvatures were measured with a
stylus profilometer DEKTAK 3030. As most commonly, the
stress in our films has been calculated by the bend-bending
method, where the radius of the bent, coated substrate is de-
termined and used to calculate the residual stress. Recently L.B.
Freund and coworkers [11] extended the use of the simplified
form of Stoney’s formula [12] to a broader class of film-substrate
configurations. In our case, we can properly assume that geo-
metrical requirements and mechanical assumptions [13] are
verified: (i) the film and the substrate thickness are small
compared to the lateral dimensions, (ii) the substrate thickness is
much greater than the film thickness, (iii) the film thickness is
uniform with good adhesion to the substrate, (vi) the stress is
isotropic, without any preferential direction, i.e., the curvature of
the substrate is uniform, and (v) the deformation both for the film
and the substrate is situated in the elastic domain. The internal
stress in the deposited film is calculate from the change in the
substrate curvature from 1/R0 for the bare substrate to 1/R(e) after
the thin film deposition, with the following Stoney’s formula:
 
Es e2s 1 1 1
r¼ 
6ð1  vs Þ e RðeÞ R0
where R0 is the radius of curvature of the bare Si substrate, R(e) is
the radius of curvature after the deposition of the film on the
substrate, Es and ís are, respectively, the Young’s modulus and
Table 1
Experimental parameters for reactive sputtering used in this work
Target Al (99.999%)
Base pressure 10− 4 Pa
Sputtering pressure 0.3 Pa
Gas mixture (10% N2–90% Ar)
Target current 100 mA
Target voltage 1000 V DC
Coil current 3A
Anode voltage 150 V
Substrate bias voltage 0–250 V
Fig. 1. Variation of residual stress of 300 nm thick AlN films versus negative
bias voltage of the substrate for two series of experiments, i.e., black dots and
open circles.
Poisson ratio of the substrate, es and e are the thickness of the
substrate and the film, respectively, equal to 350 μm and in the
300-nm range. The chemical composition of the layers was
analyzed by EDS (Energy Dispersive Spectroscopy, Oxford
System) with a 1-min collection time, at low energy (3 keV), in
order to check only a thickness of 300 nm or lower. It has been
checked that a 3-keV acceleration voltage was high enough to
quantify correctly the N content. All the measurements were
verified by WDS (Wavelength Dispersive Spectrometry, Cameca
SX 50). The structural investigations of the deposited films were
performed by IR absorption spectroscopy (FTIR spectrophot-
ometer, Biorad FTS 6000), the transmission spectra were
recorded at normal incidence in the wavelength range of
400 cm− 1 to 4000 cm− 1. In addition, X-ray diffraction (XRD)
analysis was performed at normal and grazing incidence with a
Siemens D5000 diffractometer using Cu Kα radiation (λ = 1.540
598 Å). Scanning Electron Microscopy (Jeol JSM-5900 LV)
observations were performed to determine the morphology of the
films.
3. Results and discussion
Aluminium nitride films were deposited using a triode
sputtering system. The experimental conditions were chosen for
deposition of stoichiometric AlN films, as described in previous
works [10]. The film chemical composition, checked by EDS
and WDS analysis, showed a Al/N ratio equal to 1.0 ± 0.1 for the
whole range of studied experimental conditions, and no oxygen
contamination was detected neither by EDS and WDS
techniques.
The internal stresses of the AlN films (300 nm thick) were
measured versus substrate bias. Results obtained for two series
of experiments, respectively, black dots and open circles, are
reported on Fig. 1. The good correlation between the two sets of
experiments stands for a good reproducibility of our process. In
the whole range of scanned bias, the stress is compressive.
Without bias, the films exhibit a residual stress as low as
0.5 GPa which increases drastically with substrate bias until it
reaches a maximum of 7 GPa for a negative bias voltage of
 B. Abdallah et al. / Thin Solid Films 515 (2007) 7105–7108
Fig. 2. XRD patterns of AlN films versus negative bias voltage of the substrate.
− 50 V. Then it decreases slowly for higher bias voltages (Fig.
1). Our results on compressive stress versus bias voltage and the
high level of stress obtained at − 50 V are in agreement with
those observed by Davis [14].
In order to understand such intrinsic stress variation,
structural analyses by X-ray diffraction were performed. The
XRD patterns of the deposited films exhibit two orientations, as
shown on Fig. 2. First, without bias voltage, the film is clearly
h-AlN, (002) oriented. With increasing bias voltage, a decrease
of the crystallinity of the films is observed: the (002) peak
disappears and a small peak, attributed to h-AlN (100)
orientation, appears between 2θ = 32° and 2θ = 33°. This change
of crystallographic orientation is confirmed by Infrared
Analysis in transmission mode (Fig. 3).
The IR spectra of films deposited without substrate bias
exhibit a single sharp peak centered at 675 cm− 1 associated to
the E1 mode of AlN [15], whereas the films synthesized at
negative bias voltage of 25 V and 50 V present a shoulder at a
lower wavelength. For higher voltage (− 75 V and − 100 V), an
enlargement and shift of the peak at a lower wavelength is
recorded (Fig. 3). For a negative bias voltage Vs = − 50 V, a
Lorentzian fit with two components yields two absorption
modes (Fig. 4): the E1 mode at 675 cm− 1 and a second one
around 618 cm− 1 which can be attributed to the A1 mode of h-
AlN (recorded in literature at 614 cm− 1 [15]).
Fig. 3. FTIR spectra for AlN films deposited with various negative bias voltage
of the substrate.
7107
Fig. 4. Example of a two components Lorentzian fit of the FTIR spectra obtained
for AlN film deposited for Vs = 50 V.
First, it appears that despite the relatively low substrate
temperature 400 K to 500 K, the deposited AlN films are well
crystallized (Fig. 2). In the present work, the deposition rate was
up to 1 nm/s. As explained previously, since depositions are
performed at low working pressure and according to reference
[16], the difference between the plasma potential and the
floating potential is around 30 V. Therefore, the argon and
nitrogen species have enough energy (30 eV) to favor a well-
crystallized growth without bias voltage [17]. Moreover,
Hultman et al. [18] have shown that at low pressure, energetic
neutral species constitute an important additional source of
energy and momentum at the growing film surface for
promoting densification and crystalline orientation of the film.
Second, one can see that the increase of bias voltage during
deposition process leads to an increase of the intrinsic stress and
an amorphization of the films associated with a texture change.
In the following, one may try to correlate the stress, structure
behavior of the film and the deposition conditions. On the basis
of XRD measurements, well-crystallized (002) oriented AlN
films are obtained without biasing substrate. In the present
experiments, the nitrogen to argon flow rate ratio [R = N2 / (Ar +
N2)] is equal to 10% and leads to AlN films exhibiting a (002)
preferential orientation in good agreement with work of Ishihara
et al. [19]. In fact, at such a low R flux ratio, we may consider
Fig. 5. Evolution of XRD diffraction patterns taken at a grazing incidence α = 7°
for films deposited at various negative bias voltage of the substrate.
7108 B. Abdallah et al. / Thin Solid Films 515 (2007) 7105–7108
that a partially nitrided target is involved with a metallic
sputtering regime. Therefore, we assume that the sputtered
species reaching the substrate are mainly Al and N species with
ions energy in the range of 30 eV since no bias voltage is
involved. Thus, the ion bombardment is too weak for breaking
the AlN chemical bonds on the c-axis, the most favored growth
direction is therefore (002) [20]. In addition, as the films are
well crystallized the internal stress remains relatively low. When
the negative bias voltage is increased from 50 V to 100 V, the
ion bombardment on the growing film increases and becomes
high enough to break some chemical bonds. This increase of
species bombardment becomes responsible for the lattice
damage and may explain the drastic increase of the stress and
the disappearance of the (002) orientation as observed by the
grazing incidence analysis at α = 7° (Fig. 5). For bias voltages
above − 50 V, the peak of silicon substrate is recorded on the
DRX patterns due to a re-sputtering of the films which leads to
lower thickness. Indeed, as the bias voltage increases, the ion
bombardment also increases and the stress decreases following
the model of Davis [14]. This is associated with a re-
crystallization of the film and the apparition of the (100)
orientation.
In fact, when the negative bias voltage of the substrate
reaches 150 V, the XRD measurements show that all AlN
chemical bonds on the c-axis are broken and we observe again a
crystallization of the films but with a (100) orientation. Such a
behavior during the deposition process has been already
observed for hexagonal piezoelectric ZnO thin films [21].
4. Conclusion
In this paper, we report on structural investigations and stress
measurements of AlN films deposited by a triode sputtering
system. Attempts are made to explain the film’s structural
changes that occur during the deposition process when a
negative RF bias voltage is applied to the substrate. The
compressive stress, calculated from substrate curvature, has a
relatively low value without substrate bias. The residual stress
increases and reaches a value up to 7 GPa for a negative bias
voltage of 50 V. For higher bias voltage, the compressive stress
decreases. Films deposited without bias voltage are well
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crystallized and (002) oriented despite a low deposition
temperature of 400 K. When a bias voltage is applied, an
amorphization of the film is first observed and finally a (100) h-
AlN orientation appears for a negative bias voltage of 150 V.
The structure of the AlN films and their orientation are well
correlated to the variations of compressive stress and ion
bombardment strength. The RF substrate bias appears not
suitable for depositing well-crystallized AlN films by triode
sputtering system since it is responsible for their amorphization
and a drastic increase of the internal stress.
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