Applied Surface Science 270 (2013) 225–230

Contents lists available at SciVerse ScienceDirect

Applied Surface Science

journal homepage: www.elsevier.com/locate/apsusc

Enhancement of piezoelectric response of diluted Ta doped AlN

Hongyan Liu, Fei Zeng ∗ , Guangsheng Tang, Feng Pan ∗
The Key Laboratory of Advanced Materials (MOE), Department of Materials Science and Engineering, Tsinghua University, Beijing 100084, China

a r t i c l e i n f o a b s t r a c t

Article history: The authors have investigated the variation of microstructure and piezoelectric response of Tax Al1−x N
Received 15 September 2012 films with Ta concentrations. The results indicate that moderate Ta doping facilitates the c-axis orien-
Received in revised form tation, crystallinity and enlargement of lattice constants. When the doping content is about 5.1 at.%, the
27 December 2012
c-axis orientation is optimized in the best with c constant of about 0.5086 nm. The Raman spectra of
Accepted 2 January 2013
Tax Al1−x N films further determine the wurtzite structure of AlN after Ta doping. The high resolution
Available online 9 January 2013
transmission electric microscopy demonstrates that the column single crystal was obtained with pres-
ence of nano distortion domains. The Ta 4f7/2 binding energy of Tax Al1−x N shows a shift toward lower
Keywords:
Piezoelectric response
binding energy side, indicating that the coordination configuration of Ta with N changed as Ta contents
Ta increased. A significant enhancement in piezoelectric response was obtained from 4.2 pC/N to 8.2 pC/N,
AlN which is enhanced by ca. 100%, when the Ta content arrived to 5.1 at.%. The expansion of unit cell vol-
ume and the competition between Ta and Al atoms about the coordination of nitrogen atoms, which will
enhance the internal nitrogen displacement under electric field, are proposed to be the main microscopic
origin of the enhancement of piezoelectric response.
© 2013 Elsevier B.V. All rights reserved.

1. Introduction orientation, which is an essential requirement to obtain good piezo-

Aluminum nitride (AlN) film has drawn great attention over
the past decades for its promising applications in fields of elec-
tronic, optoelectronic and piezoelectric devices owning to its
outstanding properties [1–3]. Besides, due to its excellent attributes
with high surface acoustic wave velocity (6000 m/s), high tem-
perature stability (1150 ◦ C) and compatibility with conventional
silicon manufacturing technologies, aluminum nitride has been
extensively studied as an excellent piezoelectric material for appli-
cation in electroacoustic devices such as surface acoustic wave
(SAW), bulk acoustic wave (BAW) and microelectromechanical sys-
tem (MEMS) [4–6]. More importantly, with drastically increase
in industrial demand for higher temperature and higher pressure
piezoelectric sensors to monitor furnace and reactor system [7], it
is of vital importance to develop a sensor with high operating tem-
perature. Hence, AlN has obtained widespread attention as higher
temperature and higher pressure piezoelectric sensors due to its
high temperature stability, which cannot be satisfied by traditional
piezoelectric materials such as lead zirconium titanate (PZT) with
low Curie temperature. As for applications in micro- and nano-
electronics as a piezoelectric material, it is well known that AlN
films are expected to possess a microstructure with high c-axis
∗ Corresponding author. Tel.: +86 10 62795373; fax: +86 10 62771160.
E-mail addresses: zengfei@mail.tsinghua.edu.cn (F. Zeng),
panf@mail.tsinghua.edu.cn (F. Pan).
electric response in polycrystalline AlN. However, the piezoelectric
response of AlN (ca. 5.5 pC/N) [8], even though with excellent c-axis
preferential orientation, is very low in comparison with that of ZnO
(ca. 12.4 pC/N) [9]. Consequently, it is of vital importance to explore
a new method to enhance the piezoelectric response of AlN to meet
the exigent demand.
It has been reported that the piezoelectric response of AlN films
is closely related to crystal properties, i.e., c-axis orientation, polar
distribution of grains, defects in films and so on [10,11]. The influ-
ence of various deposition conditions on piezoelectric response of
AlN films has been studied comprehensively by Morito Akiyama
and other authors [12–17]. It is also reported that traces of non-
(0 0 0 2) diffraction plane parallel to the surface of substrate can
lead to degradation of the piezoelectric response of AlN [8]. How-
ever, only slight increase of piezoelectric response was obtained.
It is known to all that alloying is one of the most efficient ways of
improving materials performance including enhancement of piezo-
electric response [18]. Recently, Akiyama reported a tremendous
enhancement in piezoelectric response of AlN up to 24.6 pC/N by
alloying with scandium [19,20], which was further verified from
a structural point of view through ab initio calculation by Ferenc
Tasnadi [21]. The electromechanical coupling and dielectric prop-
erty were also studied profoundly by alloying with Sc or B [22–25].
These methods and theory open a route for dramatic increment
in piezoelectric response of AlN film. Nevertheless, it is not so eco-
nomical for widespread application in acoustic wave devices due to
the scarce of scandium. Therefore, seeking an economical metal to

0169-4332/$ – see front matter © 2013 Elsevier B.V. All rights reserved.
http://dx.doi.org/10.1016/j.apsusc.2013.01.005
226 H. Liu et al. / Applied Surface Science 270 (2013) 225–230

replace scandium is needed based on the aforementioned method

and theory to enhance the piezoelectric response of AlN film.
The aim of this study is twofold. First, we wanted to study the
structural evolution of AlN upon alloying with tantalum and obtain
transition metal doped AlN with high quality. A series of Tax Al1−x N
films (x = 0–0.079) were deposited on (1 0 0) silicon wafers by tra-
ditional simple method of reactive co-sputtering. Second, we tried
to enhance the piezoelectric response of AlN and study the cor-
relation between piezoelectric response and the microstructure of
Tax Al1−x N films. We hope to find a new way to design AlN crys-
tal to explore its piezoelectric use requiring high performance and
stringent condition.

2. Experimental

Tax Al1−x N films were prepared on n-type Si (1 0 0) substrates by

direct current magnetron reactive sputtering at 400 ◦ C in a mix-
ture of pure argon and nitrogen gases. The target material was
aluminum with a purity of 99.999% and a diameter of 3 in. For tanta-
lum doping, a few tantalum chips were distributed uniformly on the
aluminum target and the tantalum concentration was controlled by
changing the number of tantalum chips. Prior to inserting into the
chamber, the silicon wafers, whose electrical resistivity is lower
than 0.02  cm for piezoelectric response measurements, were
ultrasonically cleaned successively in acetone and alcohol for 8 min
each and then put in diluted hydrofluoric acid to remove the sur-
face oxide, after which the silicon wafers were rinsed in deionized
water for another 5 min and dried with pure nitrogen. The sys-
tem was generally pumped down to a base pressure of 3 × 10−5 Pa,
and then high purity argon (99.999%) and nitrogen (99.999%) were
introduced with partial pressure of 0.25 Pa and 0.15 Pa, respec-
tively. Prior to each deposition, the target was cleaned in situ by
Ar+ ion bombardment for 10 min and then pre-sputtered under
the same deposition conditions for 5 min with shutter closed. The
film thicknesses were kept at ca. 600 nm which was measured by a
stylus profiler.
The crystal structure and orientation of the films were inves-
tigated by X-ray diffraction (XRD) with a Rigaku diffractometer
using mono-chromatized Cu K␣ (=1.5406 Å) radiation. The c and
a-axis lattice parameters were determined using the triple-axis
–2 scans on the (0 0 2) and (1 0 2) reflections in symmetric
and asymmetric (tilting sample by 42.5◦ ) geometries, respec-
tively. The microstructure of the sample was characterized by
high-resolution transmission electron microscopy (HRTEM). TEM
experiments were performed using JEOL-2010F operated at 200 kV.
X-ray photoelectron spectroscopy (XPS) analysis was performed to
determine the chemical state and the concentration of Ta in the AlN
matrix by Escalab 250Xi X-ray photoelectron spectrometer with Al
K␣ radiation of 1486.6 eV. The kinetic energy of the photo emitted
electrons was measured in an electron energy analyzer operated in
constant pass energy of 20 eV. The Raman measurement was per-
formed at room temperature in the backscattering configuration at
the film surface using the 488 nm line from Ar+ laser. The piezo-
electric response of the films was measured using a piezoelectric
force microscopy (PFM).
3. Results and discussion
Fig. 1(a) shows the typical XRD spectra of Tax Al1−x N
(x = 0–0.079) films with various tantalum contents deposited on Si
(1 0 0) substrate. One can observe a strong (0 0 2) peak belonging
to the diffraction pattern of hexagonal wurtzite AlN structure. No
diffraction peaks from other phases related to metallic tantalum or
clusters of tantalum nitrides were detected within the detection
limit of the XRD measurement. The strong (0 0 2) diffraction peak
Fig. 1. (a) XRD spectra of Tax Al1−x N (x = 0–0.079) films deposited on Si(1 0 0) sub-
strate. (b) Dependence of lattice constants and FWHM of rocking curve of AlN films
on tantalum contents. Closed squares, circles and rhombus indicate c-axis, a-axis
lattice parameters and FWHM of rocking curves of Tax Al1−x N (x = 0–0.079) films,
respectively.
indicates that the film has c-axis orientation normal to the surface of
the silicon substrate. Accompanying with the increased Ta contents,
the 2 position of (0 0 2) peak shifts firstly to lower angle, arrives
to the lowest value at the Ta concentration of 5.1 at.%, and then
increases reversely. The relative intensity of the (0 0 2) diffraction
peak varies with the Ta contents in the same trend. However, the
full width at half maximum (FWHM) of the rocking curve of (0 0 2)
plane behaves in a contrast style as shown in Fig. 1(b). It decreases
drastically from 4.4◦ to 2.5◦ for the sample with Ta concentration of
5.1 at.%, which is superior to that of published data [12,13,16]. These
results indicate that the preferential orientation was improved and
the crystallinity was enhanced significantly by the Ta doping, and
arrived to the optimal values when the Ta content was 5.1 at.%.
Fig. 1(b) also shows the great variations in lattice constants a
and c as a function of Ta contents. Out-of-plane lattice constant
c was calculated based on the relation c = /sin(), while in-plane
constant a was determined by the c lattice constant and d value of
the (1 0 2) plane using the following formula:
 
1 4 h2 + hk + k2 l2
= + ,
2
dhkl 3 a2 c2
where h, k, l are miller indices, c and d are lattice constants for the
(0 0 2) and (h k l) planes, respectively. It is noteworthy that the vari-
ation trend in lattice constants a and c with Ta contents resembles
with each other. In general, after doping Ta in AlN films, one would
expect larger lattice constants due to the larger atomic radius of Ta
(0.7 Å) than Al (0.5 Å), thus, for Tax Al1−x N (x = 0–0.051) films, the
lattice constants a and c increase almost linearly with Ta content.
However, as the Ta doping content exceeds 5.1 at.%, the 2 position
shifts reversely to higher angle, i.e., the lattice constants decrease
with further increase in Ta contents. These results suggest that the
Ta atoms could dissolve in the AlN crystal lattice to the maximum
 H. Liu et al. / Applied Surface Science 270 (2013) 225–230 227

Fig. 2. (a) Raman spectrum of c-axis oriented undoped AlN films on (1 0 0) silicon substrate. The peaks inidicated by asterisks are attributed to the Si(1 0 0) substrate. (b) An
enlarged view of the spectral region where the E2 (high) optical phone of AlN is visible for six samples. The two superimposed peaks were fitted by Lorentzian function to
extract the peak positions and FWHM of E2 (high) peak as shown in the right panel with dashed lines. The spectra were smoothed and have been vertically shifted for clarity.
Concentration dependence of the peak positions and FWHM of (c) E2 (high) and (d) A1 (LO) phonon of Tax Al1−x N (x = 0–0.079) films.

solid solution of about 5.1 at.%. Higher doping values would result
in precipitation of some Ta compounds and stress releasing, which
reduced the real Ta contents in AlN lattice and the lattice constants.
Raman spectroscopy and HRTEM were further performed to
provide profound assessments of the crystal structure of the
Tax Al1−x N films as well as defects or impurities. As is known to
all that, the wurtzite AlN has a hexagonal unit cell with two lattice
parameters, a and c, and belongs to the space group c64v . The struc-
ture is composed of two interpenetrating hexagonal close-packed
sublattices, each sublattice includes four atoms per unit cell and
all atoms occupying C3v sites. According to the group theory, six
optical phonon modes of A1 + 2B1 + E1 + 2E2 are predicted at the 
point of the Brillouin zone. Out of these modes, the two E2 modes,
high
denoted as E2 and E2low , are both Raman and infrared active, and
the two B1 modes are Raman silent. Since A1 and E1 mode are
polar, they can split into longitudinal optical (LO) and transverse
optical (TO), and one of A1 and E1 branch, in which the phonon is
polarized in the z direction and in x–y plane, respectively, is Raman
silent [26]. Fig. 2(a) depicts the Raman spectra of c-axis oriented
Ta0.051 Al0.949 N film on (1 0 0) silicon substrate. The peaks indicated
by asterisks are attributed to the Si (1 0 0) substrate. The peak at ca.
high
655 cm−1 corresponds to the E2 mode of the AlN, the strongest
of the allowed modes in c-axis oriented wurtzite film under the
backscattering configuration used in this experiment [26]. Another
predicted phonon for backscattering geometry measurement is
high
A1 (LO) at ∼886 cm−1 . The existence of E2 and A1 (LO) modes indi-
cates that the deposited Tax Al1−x N films are of wurtzite structure,
which is consistent with the result of XRD analysis. Fig. 2(b) shows
high
an enlarged view of the spectral region where the E2 optical
phonon of AlN is visible for the six samples. The two superimposed
peaks, centered at ∼655 cm−1 , were fitted by Lorentzian function
high
to extract the peak position and FWHM of E2 peak as shown in
Fig. 2(b). Fig. 2(c) and (d) shows the variations in peak positions
high
and FWHM of E2 and A1 (LO) of Tax Al1−x N (x = 0–0.079) films as
a function of tantalum content, respectively. From Fig. 2(c), one
high
can observe that a large blue-shift in E2 phonon frequency and
high
an augment in FWHM for the E2 phonon mode are driven by
an increase of compositional disorder, which is due to the break-
ing of translational symmetry induced by atomic substitution or by
creation of defects. As was pointed out by L. Bergman et al. [27],
the width of the peak reflects the phonon anharmonic decay, the

Fig. 3. (a) Cross-sectional TEM bright-field image of the as-grown Ta0.051 Al0.949 N film. (b) HRTEM image of an individual grain. The inset in (b) is the corresponding SAED
pattern.
228 H. Liu et al. / Applied Surface Science 270 (2013) 225–230
Fig. 4. XPS spectra of Ta 4f core-level of Tax Al1−x N (x = 0.024–0.079) films.
crystalline quality, and the presence of defects, which increases the
number of channels for phonon decay, therefore increasing the line
width. Hence, we concluded that elastic scattering due to disorder,
which was induced by the creation of defects upon Ta doping, and
the compositional inhomogeneities are the reason for the blue-shift
high
of peak position of E2 rather than the strain fields [28]. Investi-
gation of the spectral features of A1 (LO) mode can also be useful to
know the influence of Ta doping on the A bond in the (0 0 0 2) direc-
tion. We examined the peak position and FWHM value of this mode
carefully. Unfortunately, the variations of A1 (LO) phonon peak pos-
itions as a function of tantalum content were not obvious due to
its very weak intensity, which was fell in the error range as shown
in Fig. 2(d). However, an increase in the FWHM is observed with
increase in Ta contents in AlN films, suggesting increasing rates of
scattering of A1 (LO) phonons due to increase in Ta contents.
Low magnification cross-sectional TEM was used to charac-
terize the texture of the deposited films, while HRTEM analysis
was carried out to explore the lattice structure and to investi-
gate the possibility of nano-clusters or secondary phase formation.
Fig. 3(a) shows a representative low magnification cross-sectional
TEM image of the selected Ta0.051 Al0.949 N film. It reveals that the
film consists of highly parallel, columnar grains, which penetrate
through the entire film with thickness of ca. 600 nm. Fig. 3(b)
exhibits the HRTEM image of an individual grain and the corre-
sponding selective area diffraction (SAED) pattern. One can see
that the column is a single crystal with the growth direction along
[0 0 0 1]. The corresponding SAED pattern is composed of sharp dis-
crete dots corresponding to wurtzite structure, showing that the
column has a single crystalline wurtzite structure with absence of
any other phases. The interplanar spacing is 0.252 nm, resulting in a
lattice constant c of 0.504 nm which is in good agreement with that
of the XRD result, and the corresponding SAED pattern confirms
this result as well as that shown in the inset of Fig. 3(b).
Since X-ray photoelectron spectroscopy is sensitive to examine
the chemical environment of a specific element, so it was employed
to investigate the existence form of Ta in Tax Al1−x N films, which
reflects the coordination of Ta with N in some extent. The Ta 4f
core-level spectra were obtained by narrow range scanning of XPS
after 5 min of Ar+ sputtering to avoid surface contamination. All
of the spectra were calibrated with C1s of 285 eV originated from
adventitious carbon contamination. Fig. 4 shows the Ta 4f core-level
spectra of Tax Al1−x N (x = 0.024–0.079) films. As shown in the figure,
the spectra consist of Ta 4f7/2 and Ta 4f5/2 doublet with energy dif-
ference of 1.9 eV and the binding energy values of the doublet are
located in the vicinity of 23.6 and 25.5 eV, respectively, which is
in agreement with that of TaN films [29,30]. Besides, the intensity
of the doublet shows an increment with increasing Ta concentra-
tion, showing that the concentration of Ta in Tax Al1−x N films is
Fig. 5. Variation in piezoelectric coefficient d33 as a function of Ta contents.
increased. However, as can be seen from Fig. 4, the binding energy
of Ta 4f7/2 gradually shifts toward lower binding energy side from
ca. 23.6 eV to ca. 23.3 eV with increase in Ta content. The evolution
of Ta 4f7/2 binding energy indicates that the coordination configura-
tion of Ta with N was changed as Ta contents increased, indicating
the increase in the N coordination with Ta atoms inside the wurtzite
lattice.
The potential application of piezoelectric materials requires the
significant enhancement of piezoelectric response. In this work,
the piezoelectric coefficient d33 was measured using piezoelectric
force microscopy (PFM). Fig. 5 shows the variation in piezoelectric
coefficient d33 of Tax Al1−x N films as a function of Ta contents. As
shown in Fig. 5, the piezoelectric coefficient d33 of pure AlN film
is ca. 4.2 pC/N, which is substantially lower than that of bulk AlN
(5.4 pC/N) [31]. After Ta doping, the piezoelectric coefficient d33
of Tax Al1−x N films increases substantially by 93% to 8.2 pC/N at Ta
concentration of 5.1 at.%. The absolute values and the magnitudes
of enhancement in piezoelectric response are just lower than those
reported by Morito Akiyama et al. [19]. Understanding the mecha-
nism of the enhancement of piezoelectric response is important for
future designation of novel piezoelectric materials. Tasnadi et al.
using ab-initio calculation demonstrated that the giant enhance-
ment of piezoelectric response in Sc alloyed AlN films is due to the
alloy effect [21]. However, we think that there should exist promi-
nent difference in the mechanism of enhancement piezoelectric
response between the Sc-doped and Ta-doped AlN. For Sc-doped
AlN, the lattice constant varied much more greatly because of great
increase of a constant and then large decrease in the ratio of param-
eter c to a. For our Ta-doped AlN, the variation of c/a ratio is not so
obvious (shown in Fig. 1(b)), reaching a maximum at Ta content of
ca. 5.1 at.%. Another possible mechanism for the enhancement of
the piezoelectric response is the optimal of the crystalline orien-
tation. We have found previously that the Tax Al1−x N film with Ta
content of 5.1 at.% shows the best c-axis preferred orientation with
the smallest FWHM value of the rocking curve of 2.5◦ . However, the
increase of piezoelectric response due to the enhancement of c-axis
preferred orientation is limit [32]. Therefore, it seems that there are
some intrinsic factors influencing the piezoelectric response in our
Ta-doped AlN. Dileep Karanth has reported that the main effect of
electric fields in wurtzite materials is to rotate those bonds that are
non-collinear with the polar axis other than to elongate the polar
chemical bonds, and suggested that the governing factor leading to
the piezoelectric response in wurtzite materials is the ease of bond
bending [33]. This mechanism had been demonstrated and verified
experimentally in our group by doping with V in wurtzite ZnO film,
in which a giant enhancement of piezoelectric response, an order
of magnitude (110 pC/N) higher than that of pure ZnO (ca. 12 pC/N),
was obtained [18]. We also studied systematically Cr, Fe doping in
 H. Liu et al. / Applied Surface Science 270 (2013) 225–230
ZnO, and obtained consistent results [34,35]. This effect of piezo-
electric response enhancement induced by doping with other small
ions is further manifested experimentally by other groups [36]. The
mechanism, namely through promoting the rotation of the polarity
bond, is also suitable for our Ta-doped AlN.
Considering the aforementioned structural and chemical anal-
ysis, we consider that, when Ta atoms substitute for Al atoms, the
unit cell volume is expanded and the Al and Ta atoms compete
about the coordination of nitrogen due to the different coordination
configurations, thus enhancing the internal nitrogen displacement.
On the other hand, due to the introduction of Ta atoms, the Ta N
bond and Al N bond will rotate more easily under electric field
upon Ta doping. As the Ta contents increase up to 5.1 at.%, this
competition becomes more evident leading to the large enhance-
ment of piezoelectric response. This model is complementary with
that suggested in V-doped ZnO, in which the cation with smaller
size than Zn2+ is easily moved under external electrical field [18].
Though the size of Ta ions is larger than Al, the expansion of the
lattice gives the anions more space to rotate and move under elec-
tric field. However, when the Ta concentration exceeds 5.1 at.%, the
piezoelectric coefficient reduces rapidly with the further increase
in Ta concentration. Recalling the fact that the 2 position of (0 0 2)
peak shifts toward higher angle side, this means that the lattice
constants are reduced, leading to the contraction of crystal lattice.
Consequently, the piezoelectric coefficient d33 is minished due to
the contraction of crystal lattice. On the other hand, the over doping
leads to the increase in the N coordination with Ta atoms inside the
wurtzite lattice, which weaken the nitrogen displacement in AlN
matrix, hence, the piezoelectric response is reduced.
4. Conclusions
In this study, the influence of Ta doping on the microstructure
and piezoelectric response of AlN films were investigated compre-
hensively by means of XRD, Raman spectroscopy, HRTEM, XPS as
well as PFM. The c-axis preferential orientation and crystallinity
were promoted tremendously upon appropriate Ta doping, which
reveals that moderate Ta doping is beneficial for obtaining high
quality AlN films. When the doping content is about 5.1 at.%, the
c-axis orientation is optimized in the best with c constant of about
0.5086 nm. The Raman spectra of Tax Al1−x N films further deter-
mines the wurtzite structure of AlN after Ta doping, and reveals
high
a large blue-shift in E2 phonon frequency and an augment in
high
FWHM for the E2 phonon mode, which are driven by an increase
of compositional disorder due to the breaking of translational
symmetry induced by atomic substitution or by the creation of
a large amount of defects and local distorted domains. The high
resolution transmission electric microscopy demonstrates that the
column single crystal was obtained with presence of nano distor-
tion domains. The Ta 4f7/2 binding energy of Tax Al1−x N shows a
shift toward lower binding energy side, indicating that the coor-
dination configuration of Ta with N was changed as Ta contents
increased. After doping with Ta, the piezoelectric response of the
AlN films was enhanced greatly from 4.2 pC/N to 8.2 pC/N when
the Ta content was about 5.1 at.%. We propose the mechanism of
the significant enhancement of the piezoelectric response is that
the expansion of unit cell volume and the competition between Ta
and Al atoms about coordination of nitrogen atoms facilitates the
displacement of nitrogen atoms and the rotation of the Ta N bond
and Al N bond.
Acknowledgments
This work is supported by the National Hi-tech (R&D) project of
China (Grant 2012AA03Z706), the National Basic Research Program
229
of China under Grant No. 2010CB832905, and the National Natural
Science Foundation of China (Grant Nos. 50871060 and 50772055).
References
[1] Y. Taniyasu, M. Kasu, T. Makimoto, An aluminium nitride light-emitting diode
with a wavelength of 210 nanometres, Nature 441 (2006) 325–328.
[2] B. Fan, F. Zeng, C. Chen, Y. Yang, P. Yang, F. Pan, Influence of strain and grain
boundary variations on magnetism of Cr-doped AlN films, Journal of Applied
Physics 106 (2009) 073907.
[3] C. Mirpuri, S. Xu, J. Long, K. Ostrikov, Low-temperature plasma-assisted growth
of optically transparent, highly oriented nanocrystalline AlN, Journal of Applied
Physics 101 (2007) 024312.
[4] N. Komatsu, T. Satoh, M. Honjo, T. Futatuki, K. Masumoto, C. Kimura, H. Aoki,
Influence of inserting AlN between AlSiON and 4H SiC interface for the MIS
structure, Applied Surface Science 257 (2011) 8307–8310.
[5] D.T. Phan, G.S. Chung, The effect of geometry and post-annealing on surface
acoustic wave characteristics of AlN thin films prepared by magnetron sput-
tering, Applied Surface Science 257 (2011) 8696–8701.
[6] T. Aubert, O. Elmazria, B. Assouar, L. Bouvot, M. Oudich, Surface acoustic wave
devices based on AlN/sapphire structure for high temperature applications,
Applied Physics Letters 96 (2010) 203503.
[7] R. Mock, H. Meixner, A miniaturized high-temperature pressure sensor for
the combustion chamber of a spark ignition engine, Sensors and Actuators A:
Physical 25 (1990) 103–106.
[8] A. Sanz-Hervas, M. Clement, E. Iborra, L. Vergara, J. Olivares, J. Sangrador, Degra-
dation of the piezoelectric response of sputtered c-axis AlN thin films with
traces of non-(0 0 0 2) x-ray diffraction peaks, Applied Physics Letters 88 (2006)
161915.
[9] J. Christman, H. Maiwa, S.H. Kim, A. Kingon, R. Nemanich, Piezoelectric
measurements with atomic force microscopy, MRS Proceedings 541 (1998)
617.
[10] F. Engelmark, G. Fucntes, I. Katardjiev, A. Harsta, U. Smith, S. Berg, Synthesis of
highly oriented piezoelectric AlN films by reactive sputter deposition, Journal
of Vacuum Science and Technology A 18 (2000) 1609–1612.
[11] M. Akiyama, C.N. Xu, K. Nonaka, K. Shobu, T. Watanabe, Statistical approach
for optimizing sputtering conditions of highly oriented aluminum nitride thin
films, Thin Solid Films 315 (1998) 62–65.
[12] M. Akiyama, T. Kamohara, K. Kano, A. Teshigahara, N. Kawahara, Influence of
oxygen concentration in sputtering gas on piezoelectric response of aluminum
nitride thin films, Applied Physics Letters 93 (2008) 021903.
[13] T. Kamohara, M. Akiyama, N. Ueno, M. Sakamoto, K. Kano, A. Teshigahara,
N. Kawahara, N. Kuwano, Influence of sputtering pressure on polarity dis-
tribution of aluminum nitride thin films, Applied Physics Letters 89 (2006)
243507.
[14] M. Akiyama, T. Kamohara, N. Ueno, M. Sakamoto, K. Kano, A. Teshigahara, N.
Kawahara, Polarity inversion in aluminum nitride thin films under high sput-
tering power, Applied Physics Letters 90 (2007) 151910.
[15] M.A. Dubois, P. Muralt, Stress and piezoelectric properties of aluminum nitride
thin films deposited onto metal electrodes by pulsed direct current reactive
sputtering, Journal of Applied Physics 89 (2001) 6389.
[16] T. Kamohara, M. Akiyama, N. Ueno, K. Nonaka, N. Kuwano, Influence of alu-
minum nitride interlayers on crystal orientation and piezoelectric property of
aluminum nitride thin films prepared on titanium electrodes, Thin Solid Films
515 (2007) 4565–4569.
[17] H. Liu, G. Tang, F. Zeng, F. Pan, Influence of sputtering parameters on structures
and residual stress of AlN films deposited by DC reactive magnetron sputtering
at room temperature, Journal of Crystal Growth 363 (2013) 80–85.
[18] Y. Yang, C. Song, X. Wang, F. Zeng, F. Pan, Giant piezoelectric d33 coefficient
in ferroelectric vanadium doped ZnO films, Applied Physics Letters 92 (2008)
012907.
[19] M. Akiyama, T. Kamohara, K. Kano, A. Teshigahara, Y. Takeuchi, N. Kawa-
hara, Enhancement of piezoelectric response in scandium aluminum nitride
alloy thin films prepared by dual reactive cosputtering, Advanced Materials 21
(2009) 593–596.
[20] M. Akiyama, K. Kano, A. Teshigahara, Influence of growth temperature and scan-
dium concentration on piezoelectric response of scandium aluminum nitride
alloy thin films, Applied Physics Letters 95 (2009) 162107.
[21] F. Tasnadi, B. Alling, C. Hoglund, G. Wingqvist, J. Birch, L. Hultman, I.A. Abrikosov,
Origin of the anomalous piezoelectric response in wurtzite Scx Al1−x N alloys,
Physical Review Letters 104 (2010) 137601.
[22] A. Zukauskaite, G. Wingqvist, J. Palisaitis, J. Jensen, P.O.A. Persson, R. Matloub, P.
Muralt, Y. Kim, J. Birch, L. Hultman, Microstructure and dielectric properties of
piezoelectric magnetron sputtered w-Scx Al1−x N thin films, Journal of Applied
Physics 111 (2012) 093527.
[23] G. Wingqvist, F. Tasnadi, A. Zukauskaite, J. Birch, H. Arwin, L. Hultman, Increased
electromechanical coupling in w-Scx Al1−x N, Applied Physics Letters 97 (2010)
112902.
[24] R. Matloub, A. Artieda, C. Sandu, E. Milyutin, P. Muralt, Electromechanical
properties of Al0.9 Sc0.1 N thin films evaluated at 2.5 GHz film bulk acoustic
resonators, Applied Physics Letters 99 (2011) 092903.
[25] F. Tasnadi, I.A. Abrikosov, I. Katardjiev, Significant configurational dependence
of the electromechanical coupling constant of B0.125 Al0.875 N, Applied Physics
Letters 94 (2009) 151911.
230 H. Liu et al. / Applied Surface Science 270 (2013) 225–230
[26] E. McCullen, J. Thakur, Y. Danylyuk, G. Auner, L. Rosenberger, Investigation
of the occupation behavior for oxygen atoms in AlN films using Raman spec-
troscopy, Journal of Applied Physics 103 (2008) 063504.
[27] L. Bergman, D. Alexson, P.L. Murphy, R.J. Nemanich, M. Dutta, M.A. Stroscio, C.
Balkas, H. Shin, R.F. Davis, Raman analysis of phonon lifetimes in AlN and GaN
of wurtzite structure, Physical Review B 59 (1999) 12977.
[28] A. Cros, N. Garro, A. Cantarero, J. Coraux, H. Renevier, B. Daudin, Raman scat-
tering as a tool for the evaluation of strain in GaN/AlN quantum dots: the effect
of capping, Physical Review B 76 (2007) 165403.
[29] A. Arranz, C. Palacio, Composition of tantalum nitride thin films grown by low-
energy nitrogen implantation: a factor analysis study of the Ta 4f XPS core level,
Applied Physics A: Materials Science & Processing 81 (2005) 1405–1410.
[30] T. Elangovan, S. Murugeshan, D. Mangalaraj, P. Kuppusami, S. Khan, C. Sudha, V.
Ganesan, R. Divakar, E. Mohandas, Synthesis and high temperature XRD stud-
ies of tantalum nitride thin films prepared by reactive pulsed dc magnetron
sputtering, Journal of Alloys and Compounds 509 (2011) 6400–6407.
[31] J. Ruffner, P. Clem, B. Tuttle, D. Dimos, D. Gonzales, Effect of substrate compo-
sition on the piezoelectric response of reactively sputtered AlN thin films, Thin
Solid Films 354 (1999) 256–261.
[32] F. Martin, P. Muralt, M.A. Dubois, A. Pezous, Thickness dependence of the prop-
erties of highly c-axis textured AlN thin films, Journal of Vacuum Science &
Technology A 22 (2004) 361.
[33] D. Karanth, H. Fu, Large electromechanical response in ZnO and its microscopic
origin, Physical Review B 72 (2005) 064116.
[34] Y. Yang, C. Song, X. Wang, F. Zeng, F. Pan, Cr-substitution-induced ferroelec-
tric and improved piezoelectric properties of ZnCrO films, Journal of Applied
Physics 103 (2008) 074107.
[35] J. Luo, Y. Yang, X. Zhu, G. Chen, F. Zeng, F. Pan, Enhanced electromechanical
response of Fe-doped ZnO films by modulating the chemical state and ionic
size of the Fe dopant, Physical Review B 82 (2010) 014116.
[36] Y. Chen, X. Zheng, X. Feng, The fabrication of vanadium-doped ZnO piezoelectric
nanofiber by electrospinning, Nanotechnology 21 (2010) 055708.