Dielectric properties of amorphous hydrogenated silicon carbide thin films grown by

plasma-enhanced chemical vapor deposition

D. Brassard and M. A. El Khakani

Citation: Journal of Applied Physics 93, 4066 (2003); doi: 10.1063/1.1555676

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 JOURNAL OF APPLIED PHYSICS VOLUME 93, NUMBER 7 1 APRIL 2003

Dielectric properties of amorphous hydrogenated silicon carbide thin films

grown by plasma-enhanced chemical vapor deposition
D. Brassard and M. A. El Khakania)
Institut National de la Recherche Scientifique, INRS-Énergie, Matériaux et Télécommunications,
1650 Boulevard Lionel-Boulet, C.P. 1020, Varennes, Québec, Canada J3X 1S2
共Received 2 October 2002; accepted 3 January 2003兲
The dielectric properties have been determined for stoichiometric amorphous hydrogenated silicon
carbide 共a-SiC:H兲 films grown by means of the plasma-enhanced chemical vapor deposition
共PECVD兲 technique. The dielectric constant, dielectric loss, breakdown voltage, and current–
voltage (I – V) characteristics of the a-SiC:H PECVD films were systematically determined for
various film thicknesses in the 90–1400 nm range. The PECVD a-SiC:H films exhibit not only a
dielectric constant as high as 14 but also relatively high breakdown field values around 3 MV/cm.
The dielectric constant of the a-SiC:H films was found to remain almost constant over all the
investigated frequency range of 1 kHz to 13 MHz, while it decreases as the film thickness is
diminished. The analysis of the I – V characteristics of the a-SiC:H films has revealed the existence
of two different conduction mechanisms depending on the applied voltages. While exhibiting an
ohmic conduction in the low-field region 共⬍0.05 MV/cm兲, the film conduction at high fields 共⬎0.25
MV/cm兲 is dominated by the Poole–Frenkel effect. In the low-field region, the conductivity of the
a-SiC:H films was found to decrease exponentially from 10⫺10 S/cm to about 10⫺12 S/cm as the
film thickness is increased from 90 to 1400 nm. At high fields, a thermal breakdown of the a-SiC:H
films occurred at about 3 MV/cm as a consequence of thermal instabilities induced by Joule heating.
The excellent dielectric properties of the PECVD a-SiC:H films are seen to be a consequence of
their high density and low defect concentration. © 2003 American Institute of Physics.
关DOI: 10.1063/1.1555676兴

I. INTRODUCTION literature depending on the growth process and/or deposition

With the increasing performance of electronic devices,
there is a need for materials that can be used in extreme
environments where high temperature, high electrical power,
or radiation is present. Amorphous hydrogenated silicon car-
bide 共a-SiC:H兲 films combine a wide range of highly attrac-
tive properties including 共i兲 excellent thermal and chemical
stability, 共ii兲 high radiation resistance, 共iii兲 excellent hardness
and elastic modulus mechanical properties,1 and 共iv兲 high
optical transmittance 共⬃80% at the HeNe line兲.2 By taking
advantage of this unique combination of properties, we have
demonstrated that a-SiC:H films can be used as a membrane
material in the successful fabrication of x-ray masks for
proximity-printing x-ray lithography applications.2 In addi-
tion, a-SiC:H films possess interesting electronic
properties3,4 and are thus worthy of considerable interest for
many applications. Among these are Schottky diodes, op-
tothyristors, unipolar diodes, barrier/etch stop dielectric, pas-
sivation and protective coating, or coating layers for amor-
phous solar cells.4 –10 This material finds application in this
wide range of domains mainly because many of its properties
共such as optical band gap, conductivity, index of refraction,
or dielectric constant兲 can be tailored by varying the deposi-
tion conditions and processes.3– 6,11–13 Although there is a
large disparity in the properties of a-SiC:H films reported in
a兲
Author to whom correspondence should be addressed; electronic mail:
elkhakan@inrs-emt.uquebec.ca
conditions used, parameters such as the degree of hydroge-
nation, the SiuC bond density, the ratio of silicon to carbon,
the film density 共or the degree of porosity兲, and the content
of defects 共such as dangling bonds兲 have been identified as
the fundamental microstructural parameters that determine
the properties of the films.1– 4,6,14,15
While a large array of properties of a-Six C1⫺x :H films
have been extensively investigated, only few papers have
been reported to date on their dielectric properties.5,16 –19 In
the case of sputter-deposited a-SiC:H films, it has been re-
ported that the hydrogen incorporation into the films
共through deposition under a partial pressure of hydrogen兲
and/or post-annealing treatments influence not only their di-
electric constant but also their conductivity.19 On the other
hand, for plasma-enhanced chemical vapor deposited
共PECVD兲 a-Six C1⫺x :H films, grown from silacyclobutane
or methylsilane organosilicon precursors, the dielectric con-
stant was found to be in the range of 3.6 to 8.7, depending on
the particular combination used of precursor, dilution ratio,
and rf-plasma frequency.5
In this article, we report on the dielectric properties of
stoichiometric a-SiC:H films deposited by means of the
PECVD technique, from silane and methane precursors.
Various dielectric characteristics of these films including di-
electric constant, loss factor, and breakdown field were sys-
tematically determined as a function of the film thickness 共in
the 90–1500 nm range兲. In addition, the analysis of the
current–voltage (I – V) characteristics of the PECVD

0021-8979/2003/93(7)/4066/6/$20.00 4066 © 2003 American Institute of Physics

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 J. Appl. Phys., Vol. 93, No. 7, 1 April 2003 D. Brassard and M. A. El Khakani 4067

a-SiC:H films has provided useful insights on their conduc-

tion mechanisms.

II. EXPERIMENT

The a-SiC:H films were deposited on bare silicon wafers

共具100典, n type, 0.5 mm thick, 500 ⍀ cm兲 and on Pt-coated
silicon substrates for metal–insulator–metal 共MIM兲 capaci-
tors fabrication purposes. Prior to deposition, the substrates
were cleaned following a standard procedure.14 The films
were deposited by using a commercially available PECVD
reactor14 consisting of two horizontal parallel plates of 26 in.
diameter, between which CH4 and SiH4 reactant gases di-
luted in argon are decomposed by a plasma discharge. The
upper plate is capacitively coupled to the rf power through a
matching network while the lower one, onto which the sub-
strates are placed, is grounded. The rf-power density was set
at ⬃0.3 W/cm2 at a frequency of 100 kHz. 共At such a fre-
quency, the ion bombardment during film growth is more
enhanced than at the commonly used frequency of 13.56
MHz. This leads not only to a more efficient decomposition
of the stable methane molecule, but also to a higher film
densification.兲 The total gas pressure was 200 mTorr, and the
substrate temperature was set at 300 °C. Stoichiometric
a-Si0.5C0.5 :H 共a-SiC:H兲 films were achieved at a
关 CH4 兴 / 关 SiH4 兴 gas flow ratio of ⬃2.3. The composition of
the films was measured by means of x-ray photoelectron
spectroscopy 共XPS兲, while their thickness was determined
from both Detak profilometer measurements and cross sec-
tion scanning electron microscopy observations. The XPS
analysis was systematically performed both before and after
surface cleaning by 5 kV Ar ion bombardment. The 关Si兴/关C兴
atomic ratio 共of ⬃1兲 was found to be independent of both the FIG. 1. Variation of both 共a兲 relative dielectric constant and 共b兲 dissipation
factor of PECVD a-SiC:H films as a function of the frequency for various
Ar ion bombardment cleaning and the thickness of the films. film thicknesses varying from 90 to 1400 nm. The inset of 共a兲 shows the
The hydrogen content of the a-SiC:H films is of about 25 variation of ␧ ⬘ 共at 13 MHz兲 as a function of film thickness 共open circles
at. %, as determined by elastic recoil detection 共ERD兲 mea- correspond to experimental data while the solid line shows a fit of the data
surements. 共Previous ERD analyses have also shown that the by the two capacitors in series model兲.
oxygen contamination is below 1 at. % over the entire thick-
ness of the PECVD a-SiC:H films.兲2 For the purpose of this
study, film thicknesses in the 90–1400 nm range were inves- MHz兲 frequency range 共no bias voltage was applied and the
tigated. The deposition rate of the PECVD a-SiC:H films oscillation voltage was set at 0.05 V兲. Before each measure-
was 2.9 Å/s. The a-SiC:H film density was measured by ment, a calibration was performed to remove the parasite
weighting the 3 in. diameter Si wafers before and after the series resistance. On the other hand, a computer-controlled
a-SiC:H deposition using a microbalance, and found to be of HP4140B unit was used to measure the I – V characteristics
(2.5⫾0.2) g/cm3 for the 1.4 ␮m thick films. 共No accurate of the a-SiC:H films in the 共0–100兲 V range 共the delay time
density measurements could be performed with this method between two successive measurements was set to 1 s兲. For
for the thinner films because of the limited amount of breakdown voltage measurements, a high voltage source
a-SiC:H material to be weighted.兲 共Fluke 415B兲 was used as a power supply and a 30 k⍀ re-
For dielectric measurement purposes, MIM capacitors sistance was placed in the series with the capacitor.20
consisting of a Si/SiO2 /Ti/Pt/a-SiC:H/Pt multilayer struc-
tures were fabricated. 共The Pt top contacts were about 50 nm III. RESULTS AND DISCUSSION
thick and their area was 1.8⫻10⫺3 cm2 .) Thin probe wires
A. Dielectric characteristics
共0.1 mm diameter兲 were used to connect the capacitors to
external apparatus. The measurements were performed at Figure 1 shows typical results for the relative dielectric
room temperature and under a dark environment to prevent constant (␧ ⬘ ) and the dissipation factor (tan ␦⫽␧⬘/␧⬙, where
the ambient light to affect the electrical characteristics of the ␧⫽␧ ⬘ ⫺i␧ ⬙ is the complex dielectric constant兲 of the
films. 共In fact, the results were later found to be independent PECVD a-SiC:H films as a function of the applied frequency
of light exposure.兲 The variation of the complex impedance for various film thicknesses. It is clearly shown that both the
was measured with an HP4192a analyzer in the 共1 kHz–13 dielectric constant and the dissipation factor of the a-SiC:H
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 4068 J. Appl. Phys., Vol. 93, No. 7, 1 April 2003 D. Brassard and M. A. El Khakani

films are thickness dependent. Indeed, the high-frequency 共at

13 MHz兲 value of ␧ ⬘ is found to increase from about 8 to 14
as the film thickness is increased from 90 to 1400 nm. Con-
versely, their dielectric loss decreases as the film thickness is
increased. Similar results have been also observed in the case
of pulsed laser deposited SrTiO3 ferroelectric films.21 Such a
thickness dependence for both the dielectric constant and the
dissipation factor can be caused by the presence of either an
electrode barrier layer at the metal–dielectric interface22 or
an interfacial layer with poor dielectric properties.21 Since
the dielectric constant of our films did not show any signifi-
cant variation with frequency, neither electrode barrier-layer
effects22,23 nor defect hopping24 can be invoked to explain
the observed thickness dependency of dielectric characteris-
tics. On the other hand, our results can be reasonably ex-
plained if we assume the presence of a contamination layer
of constant thickness with dielectric properties poorer than
those of the bulk a-SiC:H films. 共This layer could result from
either or both of surface contamination due to postdeposition
air exposure and microstructural considerations such as the
effect of the termination of the material structure.兲 Indeed, FIG. 2. Leakage current density vs electrical field in a log–log plot for
the inset of Fig. 1共a兲 shows how the variation of ␧ ⬘ as a PECVD a-SiC:H films of different thickness. The inset shows the variation
function of film thickness can be fairly well described by of the conductivity ( ␴ ⫽J/E), as determined in the low-field region (E
⬍0.05 MV/cm), of the a-SiC:H films as a function of their thickness.
considering that the studied a-SiC:H-based capacitors consist
of two capacitors in series where the first capacitor repre-
sents the bulk a-SiC:H film and the second one is due to the
presence of a contamination layer.21,25,26 A reasonable fit PECVD a-SiC:H films. In particular, the decrease of the dis-
关solid line of the inset of Fig. 1共a兲兴 of our experimental data charge rf frequency from 13.56 MHz to 125 kHz has been
was obtained for a contamination layer having a thickness of shown to increase the dielectric constant of the PECVD
50 nm with ␧ ⬘ of 4 and a bulk dielectric constant of the a-Six C1⫺x :H films from 5.6 to 8.7.5 This suggests that film
PECVD a-SiC:H films of about 15. It is worth noting that densification induced by ion bombardment 共which is favored
this latter value is quite consistent with the value measured at low rf frequencies as in the case of the present study where
for 1400 nm thick films (␧ ⬘ ⫽14) where the contribution of a the films are grown at 100 kHz兲 improves the dielectric prop-
contamination layer is expected to be negligible. Another erties of the a-SiC:H films. These excellent dielectric prop-
possible interpretation of the observed thickness dependence erties of our PECVD a-SiC:H films seem most likely to be a
of the dielectric constant of our a-SiC:H films would be a consequence of their high density 共i.e., 2.5 g/cm3 which is
variation of their density with the thickness. 共For example, extremely high for a-SiC:H films兲.12,29
the dielectric constant of silica aerogel films has been shown
to scale linearly with the film density兲.27 As above-outlined
B. Current–voltage characteristics
in the experimental section, the weighting method does not
allow direct and accurate density measurements for the thin- Figure 2 shows typical variation curves of the leakage
ner a-SiC:H films and, consequently, no direct comparison current density 共J兲 as a function of the applied electric field
can be made between the thickness dependences of ␧ ⬘ and 共E兲 for the different thicknesses of the PECVD a-SiC:H
film density. However, we have demonstrated in a previous films. By presenting the data in a log–log plot 共Fig. 2兲, two
work,15 by means of Fourier transform infrared analyses, that different behaviors depending on the applied field can be
the SiuC bond density of our PECVD a-SiC:H films is clearly distinguished. First, there is a low-field region (E
reduced by a factor of ⬃2 共from 8.4 to ⬃4.0 ⬍0.05 MV/cm), where J versus E follows a linear relation-
⫻1022 bonds/cm3 ) when the film thickness is diminished ship with a slope of 1, indicating thereby that the ohmic
from 970 nm to 150 nm. This clearly indicates that the den- conduction is the dominant mechanism in this region 共such a
sity of thinner films 共⬍1 ␮m兲 should be lower than that of behavior was also observed for sputtered a-SiC:H films
thicker films 共i.e., 1.4 ␮m兲. Thus, such a film density varia- when the applied fields were lower than E⬍0.02 MV/cm,
tion 共which is a consequence of microstructural changes that and was attributed to hopping of electrons from one state to
occur in the a-SiC:H films when their thickness is varied another兲.18,30,31 In this region of low fields, the conductivity
from 0.1 to 1 ␮m兲 would also be a plausible explanation for of the films was deduced and found to be thickness depen-
the thickness dependence of the dielectric constant of the dent, as is clearly shown in the inset of Fig. 2. Indeed, it
a-SiC:H films. decreases exponentially from ⬃10⫺10 to ⬃10⫺12 S/cm when
By comparing the dielectric constant of our PECVD the a-SiC:H film thickness is increased from 90 to 1400 nm.
a-SiC:H films to literature values,5,19,28 it appears that the Such a thickness dependency for the conductivity corrobo-
value of ␧ ⬘ ⫽14 is the highest value ever reported for rates with the above-proposed interpretation of the dielectric
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 J. Appl. Phys., Vol. 93, No. 7, 1 April 2003
FIG. 3. Typical J vs E data of the a-SiC:H films presented in the 共a兲
Schottky plot 关 ln(J) vs E 1/2] and 共b兲 Poole–Frenkel plot 关 ln(J/E) vs E 1/2].
The graphs shown here are for the 350 nm thick a-SiC:H films. For this film
thickness, SE yields a dielectric constant value of 2.2, while a value of 9.2
can be deduced from the PFE by using a compensation factor 共r兲 of 1.2.
properties which assumes the presence of a higher relative
concentration of impurities and/or defects in the thinner
films.
At higher fields, the variation of J as a function of E is
quite nonlinear. Such a behavior can be explained by differ-
ent conduction mechanisms such as Schottky emission 共SE兲,
Fowler–Nordheim injection, Poole–Frenkel effect 共PFE兲,
space-charge-limited currents, and Hill’s law.32,33 Our inves-
tigations have revealed that, at a first sight, both SE and PFE
can be invoked to describe the observed J – E behaviors at
high fields. Indeed, Fig. 3 shows that a straight line is ob-
tained not only in the case of SE but also in the PFE plot for
fields higher than 0.25 MV/cm. This is not surprising since it
is known that under most circumstances experimental data
can be plotted as good straight lines on either types of
graphs, even if both models describe completely different
conduction processes.32,34 In order to discriminate between
these two mechanisms, it is worth recalling that the SE
model is derived from the thermionic emission from a metal
electrode into the conduction band of a dielectric, and J as a
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D. Brassard and M. A. El Khakani 4069
function of E is given by the following expression:32 J
⫽C exp关1/kT (e 3 E/4␲ ␧ d ␧ 0 ) 1/2兴 , where C is a temperature
dependent constant and ␧ d is the dynamic dielectric constant
of the material. On the other hand, PFE accounts for thermi-
onic emission from traps in the bulk of the insulator, and in
this case J⫽ f (E) is given by:34 J⫽CE exp关1/kTr
⫻(e 3 E/ ␲ ␧ d ␧ 0 ) 1/2兴 , where r is a compensation parameter
ranging from 1 to 2 depending on the position of the Fermi
level in the band gap.23,34 In other words, the difference be-
tween PFE and SE mechanisms is that the former is a bulk
controlled process while the latter is electrode controlled. A
reliable method to distinguish between the two models is the
electrode dependence of SE. Indeed, the current characteris-
tics of a MIM device using bottom and top contacts made
with metals of different work functions will be highly asym-
metric with the voltage polarity for the SE and symmetric for
the PFE.34 In our case, no asymmetry was observed in the
I – V characteristics of the a-SiC:H-based MIM capacitors
when two different electrodes were used 共i.e., Pt as bottom
electrode and W probe wire as a top electrode兲 and the volt-
age sign was inverted. This is a clear indication that PFE is
the dominant conduction mechanism in our PECVD a-SiC:H
films in the high-field region (E⬎0.25 MV/cm). Moreover,
␧ d values deduced from the slopes of the linear region of the
SE graphs 共i.e., ␧ d in the 1.7–2.5 range兲 are inconsistent with
the dielectric constant values measured in the previous sec-
tion. On the other hand, the PFE graphs yield ␧ d values that
equal those measured at the highest frequency in Fig. 1, with
the respective compensation factor 共r兲 values of 1.5, 1.2, 1.2,
and 1.0 for 90, 350, 700, and 1400 nm thick a-SiC:H films.
The higher compensation factor for thinner films is more
likely a consequence of a larger amount of carrier traps
and/or defects,23,34 which is, in turn, very consistent with the
presence of a surface contamination layer of which contribu-
tion is expected to decrease with film thickness. These results
provide evidence that the current of our PECVD a-SiC:H
films is bulk limited and their conduction mechanism, in the
high-field region (E⬎0.25 MV/cm), can be fairly well de-
scribed by the PFE.
C. Breakdown voltage measurements
Figure 4 shows typical I – V breakdown behavior of our
PECVD a-SiC:H films. 共As previously mentioned, break-
down voltage measurements were carried while placing a
resistance of 30 k⍀ in series with the a-SiC:H-based MIM
capacitors兲. When the capacitors are approaching their break-
down voltage, the leakage current through the dielectric be-
gins to increase more rapidly than that predicted by the PFE.
It eventually reaches a point where the voltage applied to the
capacitor cannot be further increased and the I – V curve
starts to bend 共see Fig. 4兲. Such a behavior has been already
observed for silicon oxide films and was attributed to the
thermal instability created by Joule heating of the
dielectric.20,35 The Joule heating increases the temperature
and, consequently, the conductivity of the dielectric material.
When the resistance of the capacitor thus decreases, the 30
k⍀ series resistance acts like a voltage divider and reduces
the capacitor voltage, which explains the bend observed in
 4070 J. Appl. Phys., Vol. 93, No. 7, 1 April 2003
FIG. 4. Typical I – V curves of the a-SiC:H MIM capacitors where the
applied voltage is increased until the occurrence of film breakdown. 共The
curve shown here is for the 1400 nm thick a-SiC:H films.兲 The inset plot
shows the variation with thickness of the breakdown voltage of the a-SiC:H
films.
Fig. 4. Such a bend in the I – V curve is a signature of the
onset of what is qualified as a thermal breakdown, an effect
which has been reported to depend only on the insulator
properties.20 It is worth noting that the power dissipated in
the films at the maximum voltage was found to be as high as
107 W/cm3 , which is two orders of magnitude higher than
the values reported for silicon oxide films.20 This high value
indicates that these PECVD a-SiC:H films possess an excel-
lent thermal resistance and their breakdown occurs only un-
der extreme conditions.
The data displayed in the inset of Fig. 4 shows that the
breakdown voltage of the a-SiC:H films linearly increases
with the film thickness. 共It increases from 30 to 420 V when
the thickness of the films is increased from 90 to 1400 nm.兲
The slope of the straight line that fits these data yields an
average breakdown field of these a-SiC:H films of (3.1
⫾0.2) MV/cm. 共The 90 nm thick films, where the surface
layer plays a greater role, exhibited a slightly higher break-
down value 共⬃3.3 MV/cm兲 in comparison to the thicker
films.兲 These breakdown fields are much higher than the very
few values reported for a-Six C1⫺x :H films, values which are
in the 0.6 –1.0 MV/cm range.16,17 The higher density of our
a-SiC:H films 共i.e., their lower degree of porosity兲 seems
likely to be the reason for their high breakdown voltage.
IV. CONCLUSION
The dielectric properties together with the conduction
mechanism of PECVD stoichiometric a-SiC:H films have
been investigated. These films exhibit excellent dielectric
properties 共i.e., a dielectric constant as high as 14 together
with a relatively high breakdown field of about 3 MV/cm兲.
This desirable dielectric behavior of the a-SiC:H films is
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D. Brassard and M. A. El Khakani
thought to be due to their high density and very low concen-
tration of defects 共for the 1400 nm thick films the compen-
sation factor 共r兲, which reflects the level of defects, is at its
lowest value of 1兲. The lowering of the dielectric properties
of the a-SiC:H films as their thickness is decreased, from
1400 to 90 nm, is thought to be due to either or both of the
presence of a surface contamination layer with poorer dielec-
tric properties and thickness dependence of the film density.
By analysing the J – E characteristics of the a-SiC:H films,
we were able to determine that the electrical conduction
mechanism is bulk limited, being characterized by an ohmic
conduction at low fields (E⬍0.05 MV/cm) and by the PFE
at high fields (E⬎0.25 MV/cm). Finally, it is shown that the
a-SiC:H films can sustain very high levels of dissipated
power 共about 107 W/cm3 ) before their breakdown 共which
occurs at breakdown fields as high as 3 MV/cm兲. This ther-
mal breakdown is believed to be a consequence of thermal
instabilities induced by Joule heating.
ACKNOWLEDGMENTS
This work was financially supported by the Natural Sci-
ence and Engineering Research Council 共NSERC兲 of Canada
and MICRONET 共Network of centers of excellence on mi-
croelectronic devices, circuits, and systems for ULSI兲.
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