IEEE SENSORS JOURNAL, VOL. 19, NO.
12, JUNE 15, 2019
Vertically Aligned Carbon Nanotubes
Capacitive Sensors
Siva K. Reddy, Itay Gendelis, and Assaf Ya’akobovitz
Abstract— Capacitive sensors are key components in a wide
range of sensing applications, such as gas detectors and safety
systems. While the mainstream silicon sensors demonstrated good
performances, vertically aligned carbon nanotubes (VA-CNTs)
outperform them and, therefore, are an attractive candidate
material for capacitive applications owing to their extremely high
surface area. Specifically, their top (crust) layer is characterized
by a porous and dense morphology that further enhances
the capacitive area and, consequently, induces an electrostatic
fringe field and an enhancement of the capacitance. In this
paper, we study how the porosity of VA-CNTs determines their
electrostatic behavior. We observed that the porous surface of the
crust layer generates a significant enhancement of the capacitance
comparing to parallel plate capacitors. The rough surface of
the crust layer results in amplification of the VA-CNT effective
capacitor area, which further increases with the electrostatic
gap. As-grown VA-CNTs with lower porosity demonstrate higher
capacitance; however, densified samples and samples reinforced
with conductive nano-particles did not show an enhancement
of the capacitance, due to a significant change in their CNT
formation. Thus, this paper emphasizes the influence of the
morphological structure of VA-CNTs on their capacitance and
enriches the material library that can be used for capacitive
sensing.
Index Terms— V-shaped MEMS devices, thermal MEMS, tem-
perature sensors.
I. I NTRODUCTION
D UE to their high performances, miniaturized size and
compatibility with integrated circuit (IC) technology,
capacitive sensors have shown increasing popularity in scien-
tific and industrial systems. These include capacitiave micro-
accelerometers [1], proximity sensors [2], robotic sensory
skin [3], and more [4], [5]. Emerging technologies, such as
wearable electronics, autonomous robots, and the internet of
things (IoT) [6], will further increase the demand for multiple
small-size and accurate sensors that will be embedded in
engineering systems. This, therefore, requires the development
of new sensing materials that can further improve the per-
formance of such sensors and open new frontiers for future
sensors.
Manuscript received November 20, 2018; revised February 7, 2019;
accepted February 9, 2019. Date of publication February 13, 2019; date
of current version May 16, 2019. This work was supported by the Israeli
Ministry of Science and Technology under Grant 53253. The associate editor
coordinating the review of this paper and approving it for publication was
Prof. Bhaskar Choubey. (Corresponding author: Assaf Ya’akobovitz.)
The authors are with the Department of Mechanical Engineering,
Ben-Gurion University of the Negev, Beer-Sheva 84105, Israel (e-mail:
assafyaa@bgu.ac.il).
Digital Object Identifier 10.1109/JSEN.2019.2899060
1558-1748 © 2019 IEEE. Personal use is permitted, but republication/redistribution requires IEEE permission.
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4375
Vertically aligned carbon nanotubes (VA-CNTs) are one of
the most interesting nano-materials known today. VA-CNTs
comprise of billions of individual carbon nanotubes (CNTs)
arranged in a highly dense and oriented formation. Recent
studies reported on their unique physical properties, such
as high mechanical compliance [7] and excellent electrical
and thermal conductance [8]. These properties in conjunc-
tion with nano-fabrication processes compatibility, photolitho-
graphically definable geometry and high material capacitance
[9], have led to successful integration of VA-CNTs as capac-
itors in wide range of applications. For instance, VA-CNTs
were integrated into nano-scale electromechanical switches
[10] and physical sensors [11].
While the main stream silicon based capacitive sensors
demonstrated excellent performance, e.g., as proximity [3]
and motion sensors [12], their porous counterparts presented
enhanced performances due to higher surface area. These
include, for example, porous humidity sensors [13] and gas
detectors [14]. VA-CNTs, on the other hand, hold even a
greater potential to operate as capacitive devices, as they have
an extremely high surface area that exceeds that of porous
silicon. A plethora of VA-CNT based capacitive devices has
been reported and include varactors for application of electro-
static forces [15], micro-electromechanical (MEMS) vertical
comb-drive electrodes [16], electrostatic switches [10], force
and strain sensors [17], and biosensors [18].
The porous morphology of VA-CNTs induces an electrosta-
tic fringe field when subjected to voltage. Fringe fields have
been throughly investigated in many micro-scale devices, e.g.
MEMS beams [19], plates [20], perforated elements [20], and
comb-drives [21]. Our recent work has shown that the unique
fibrous microscopic structure of VA-CNTs results in sidewall
capacitive area significantly larger than a flat surface capacitor
having the same dimensions [9].
Despite the extensive research on VA-CNT capacitive
devices and the multiple reported applications, the influence
of the crust layer porosity on their capacitive behavior has
remained uncovered. In this work, we bridged this gap by
studying the porosity dependent electrostatic capacitive behav-
ior of the VA-CNTs crust layer.
II. M ETHODS
A. Samples Preparation
VA-CNT were grown by chemical vapor deposition (CVD)
process at atmospheric pressure. Silicon wafers with 1000 nm
thermal oxide were used as the substrates. The substrates were
4376 IEEE SENSORS JOURNAL, VOL. 19, NO. 12, JUNE 15, 2019

Fig. 1. CVD recipe for VA-CNT growth. (a) Gases flow rates. (b) Temperarure.

prepared by cleaning and e-beam evaporation of Fe (1.2 nm)

and Alumina (10 nm). The CVD process started with steps
of purging and preparation of the environment prior to the
growth. Next, we raised the temperature to growth temperature
(750o C), during which we also annealed the catalyst. Then we
grew the VA-CNTs by maintaining the growth temperature
while flowing 100 sccm of C2 H4 (carbon source) and H2
(reduction gas), and 400 sccm of He for 30 minutes. Finally,
the C2 H4 flow was stopped and the samples were cooled back
to room temperature, Fig. 1. The recipe shown in Fig. 1 was
used in our previous publications [22], [23], although many
other recipes have been suggested in the literature and yielded Fig. 2. SEM images of a VA-CNT sample. (a) Isometric view (scale-bar is
VA-CNTs with similar heights and morphologies [24]–[27]. 10 μm). (b) Enlarged isometric view of the crust layer (scale-bar is 500 nm).
(c) Top view of the crust layer (scale-bar is 1 μm).
The high temperatures of the CVD processes and the dominant
van-der Waals interactions between adjacent CNTs dictate
their aligned formation, without the need to apply external
forces [28], [29].
A high resolution scanning electron microscope (HR-SEM)
images of a VA-CNT sample are shown in Fig. 2. These
images show that the average distance between the CNTs
is ∼60 nm. Raman spectrum of one of our samples is shown
in Fig. 3a and demonstrated clear D- and G-band peaks that
are both characteristics for VA-CNTs. The G-band is a first
order vibrational Raman mode that corresponds to tangential Fig. 3. (a) Raman spectrum of VA-CNT sample. D- and G-bands are clearly
observed. (b) TEM image of CNTs. An average diameter of 15 nm was
vibration of sp2 carbon atoms [30]. The D-band is a disorder extracted for the CNTs.
induced band, which comes from a second order scattering
process and provides information on structural defects and
B. Experimental Setup
presence of crystalline disorder. An average diameter of the
individual CNTs of 15 nm was extracted from transmission A custom-built setup was used to acquire the electrosta-
electron microscope (TEM) images, Fig. 3b. The porosity tic gap (i.e., distance between the samples and an elec-
of our samples was acquired by image processing of top trode) dependent capacitance of the samples, as illustrated
view HR-SEM images (Fig. 2c). The porosity is defined in Fig. 4(a). This setup includes a vertically movable flat
here as the volume not occupied by the CNTs, i.e., voids conductive electrode, which is connected to an LCR meter
volume. (Keysight E4980A). The position of the electrode with respect
REDDY et al.: VA-CNTs CAPACITIVE SENSORS
Fig. 4. (a) Illustration of the experimental setup. (b) Capacitance measure-
ments of as-grown VA-CNT samples having different values of porosity. The
capacitance of a flat capacitor is shown as square yellow markers.
to the VA-CNT samples was controlled by a computer through
a LabView interface that was also used to save the capac-
itance data. Each capacitance measurement we show below
was obtained by averaging 10 cycles, on each cycle the tip
was approaching closer to the samples (during which the
capacitance data was acquired) and then returned back to its
initial position. These measurement cycles demonstrate low
distribution (i.e., small values of the standard deviation), which
is shown in Fig. 4(b) as error bars. No hysteresis was observed
when comparing the measurement cycles.
III. R ESULTS AND D ISCUSSION
Capacitance measurements as a function of the gap between
the flat electrode and the samples is shown in Fig. 4(b) for
several as-grown samples having porosity between 8.0% to
27.3%. Additionally, the capacitance measurement of a flat
paralle plate capacitor, acquired by measuring the capaci-
tance of a plain highly doped silicon chip, is also shown
in Fig. 4(b) (square yellow markers) and presented capacitance
significantly lower than that of all as-grown VA-CNT samples.
Our capacitance measurements show that samples with lower
porosity (namely, that their crust layer is occupied by more
CNTs) have higher capacitance. This is further emphasized
in Fig. 5, where the relative increase of capacitance comparing
to a flat capacitor (namely, C = C V A−C N T − C f lat , where
C V A−C N T and C f lat are the capacitances of the VA-CNTs
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Fig. 5. Relative capacitance enhancement as a function of the porosity for
gaps of 169 μm (blue squares), 259 μm (red asterisks), 500 μm (yellow
stars), and 900 μm (purple triangles).
and a flat capacitor, respectively) of several fixed gaps are
presented. Those measurements show that the capacitance
of as-grown VA-CNTs significantly exceeds that of a flat
capacitor. Under high values of porosity (15-30%) the increase
in capacitance is between 5-30%, while samples with lower
values of porosity, i.e. porosity smaller than 15%, showed even
a greater capacitance increase of several tens of percentages
that, in some cases, even exceeds 100%.
Theoretically, the capacitance is derived from the solution
of the electrostatic boundary value problem for the potential
and obeys the following geometrical relationship [31]
0 r A
C= (1)
g
Here 0 and r are the dialectic permittivity of vacuum and the
relative dialectic permittivity of air, respectively. The capacitor
area and the gap are denoted as A and g, respectively. While
in the classical case of parallel plate capacitor the area A
is simply the area of the capacitor, in our case, the as-
grown VA-CNT capacitors have an effective area that reflects
their porosity and the fact that an electrostatic fringe field is
induced. Thus, by replacing the area, A in Eq. (1), by the
effective capacitive area of the investigated samples, Ae f f ,
we can derive the term for the latter as
Cg
Ae f f = (2)
r 0
where C is the measured capacitance and g is the gap shown
in Fig. 4(a).
The enhancement of the capacitive area, defined as the ratio
between the VA-CNT effective area (Eq. (2)) and the area of a
flat capacitor having the same in-plane dimensions, is shown
in Fig. 6 as a function of the gap. These results demon-
strate that the porosity of crust layer induces a significant
enhancement of the capacitive area, which further increases
with the gap. This observation can be explained by the fact
that the porous crust layer of the VA-CNTs has multiple CNTs
that effectively increase the capacitive area. This is also in
agreement with other works that have demonstrated that rough
4378
Fig. 6. The ratio between the effective capacitor area of VA-CNTs and the
area of a flat capacitor, as a function of the gap between the electrodes. The
electrostatic force for 1 V is shown in the inset. The electrostatic force of a
flat capacitor is shown as a yellow line.
Fig. 7. (a) SEM images of a densified VA-CNT sample (scale-bar is 100 μm).
(b) Top view of the densified crust layer (scale-bar is 100 nm). (c) Side view
of a sample densified and reinforced with gold nano-particles (scale-bar is
100 nm).
surfaces present enhanced capacitance [31] that was further
increased with the gap [32]. In addition, samples with lower
porosity demonstrated higher values of enhancement, as these
samples have more CNTs in the crust layer, such that the
electrostatic fringe field is more dominant.
The electrostatic force between the VA-CNTs and the elec-
trode is
r 0 Ae f f V 2
FE S = (3)
2g 2
The electrostatic force under a voltage of V = 1 V is shown
in the inset of Fig. 6. This force is proportional to V 2 , and
consequently, when a voltage in the order of several tens of
Volts is applied (as commonly done in MEMS devices), then
the relatively small force (nano-Newton) shown in the inset
of Fig. 6 can be increased by several orders of magnitude.
Analyzing the electrostatic force show, again, an amplification
comparing to a flat capacitor (yellow line in the inset of Fig. 6),
due to the induced fringe field.
As low porosity samples demostrated enhanced capacitance,
we densified several samples in order to further reduce their
porosity. Densification was carried out through immersing
the samples in a liquid to generate capillary densification of
IEEE SENSORS JOURNAL, VOL. 19, NO. 12, JUNE 15, 2019
Fig. 8. Capacitance measurements of (a) densified samples and (b) densified
samples reinforced with gold nano-particles. The capacitance of representative
as-grown VA-CNTs (black and green circle markers) and a flat surface (yellow
squares) are shown as a reference.
the CNTs [33]. SEM images of these samples are shown
in Fig. 7(a) and (b). In addition, other samples were densi-
fied and reinforced with conductive spheres through wetting
them with a liquid containing gold nano-particles, Fig. 7(c).
Image processing analysis reveals that crust layer porosity of
densified samples was reduced to 6% or less, namely lower
than the as-grown samples.
Capacitance measurements were then conducted on the
denfsified samples (Fig. 8(a)) and samples reinforced with
conductive spheres (Fig. 8(b)). Although as-grown samples
show that lower porosity is correlated with higher capacitance
(Fig. 4(b)), similar measurements conducted on the densified
samples show that they do not present an enhancement of the
capacitance. The densification process of the samples creates
voids and increases the samples sidewall area exposed to the
electrode on the expanse of the crust layer area, as shown
in Fig. 7(a). The sidewalls demonstrate higher porosity com-
pared to that of the crust layer, and thus, they have lower
capacitive area. In addition, the electrostatic gap between the
sidewalls and the electrode is larger than that of the crust layer.
As a result, the capacitance of the densified samples is no
REDDY et al.: VA-CNTs CAPACITIVE SENSORS
longer dominated solely by the crust layer and consequently,
demonstrates comparable capacitance values to that of a flat
capacitor.
The crust layer is formed at early phases of the synthesis
process of VA-CNTs [29]. During those early stages of the
growth, the relatively short CNTs interact with each, creating a
dense and entangled layer of CNTs that support each other and
enable the subsequent formation of vertically aligned structure
of the CNTs and the characteristic extremely high aspect ratio
of VA-CNTs [28]. Despite the fact that the crust layer is
relatively thin, it was found to influence the physical properties
of VA-CNTs. For examples, its influence over the mechanical
properties of VA-CNT samples was studied [34]. Other work
has shown that the crust layer has a profound impact on the
electrical conductance of VA-CNTs [35]. Thermally, the crust
layer showed relatively high values of negative expansion
coefficient, which is different from that of other portions [22].
We show here that the crust layer has a dominant impact
on the capacitive behavior of as-grown VA-CNTs. The fact
that this layer comprise of densely packed entangled CNTs
results in significantly higher capacitance area and dominant
electrostatic fringe field. Interestingly, these insights are com-
plimentary to other works that studied the interplay between
electrostatic fields and the hierarchical structure of VA-CNTs,
e.g., it was shown that the electrostatic field can modify
the formation of the CNTs by changing their alignment and
interaction sites [23]. However, these works did not investigate
the unique porosity dependent capacitive properties of the crust
layer. While in a previous publication it was observed that
VA-CNT sidewall capacitance outperforms flat capacitors only
at relatively large gaps (hundreds of microns or more) [9], here
we show that the crust layer demonstrates higher capacitance
than flat capacitors at all gaps including small gaps - a property
that is highly attractive for capacitive sensors.
IV. C ONCLUSION
To conclude, in the present work we have investigated the
capacitance of VA-CNTs. The influence of the porosity of
VA-CNTs on their capacitance was studied. The porosity of
VA-CNTs was acquired by means of image processing of
HR-SEM images, followed by their capacitance measurements
and analysis. Our investigation has shown that due to the high
porosity of as-grown VA-CNTs, they demonstrate significant
electrostatic fringe field and enhanced capacitance, which stem
from the dense CNT formation of the crust layer. An attempt
to further reduce the porosity of the samples through their
densification, altered their structure and resulted in reduced
crust layer capacitive area. As a result, densified samples did
not exhibited capacitance enhancement.
Our analysis shows that as-grown VA-CNTs can be used as
a core material for high-accuracy capacitive sensors, as they
show superior performances comparing to flat capacitors.
The enhanced capacitance in conjunction to other attractive
properties, such as its high mechanical compliance and com-
patibility with micro-fabrication processes, make VA-CNTs
an ideal material to be used in future miniaturized high-
end capacitive sensing applications. Therefore, VA-CNT is
4379
attractive to be integrated in emerging technologies that require
multiple small-size and accurate capacitive sensors, such as
IoT and automative systems.
ACKNOWLEDGMENT
The authors thank Dr. Oriel Shoshani for his helpful advice.
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Siva K. Reddy received the Ph.D. degree from the Indian Institute of Science,
Bengaluru, India. He has worked on the mechanical behavior of CNT and
Graphene foams. Earlier, he was working as a Research Engineer at the
Masdar Institute of Science and Technology, Abu Dhabi, in collaboration
with the Massachusetts Institute of Technology, Cambridge, MA, USA. He
is currently a Post-Doctoral Fellow with the Department of Mechanical
Engineering, Ben-Gurion University of the Negev, Beersheba, Israel, under
the supervision of Dr. A. Ya’akobovitz.
Itay Gendelis received the B.Sc. and M.Sc. degrees in mechanical engineering
from Ben-Gurion University of the Negev, Israel. His research interests include
electrostatic fields in NEMS devices and CNTs.
Assaf Ya’akobovitz received the B.Sc., M.Sc., and Ph.D. degrees in mechan-
ical engineering from Tel-Aviv University, Tel Aviv, Israel, in 2006, 2007,
and 2012, respectively. From 2012 to 2013, he was a Post-Doctoral Fellow
with the Department of Mechanical Engineering, University of Michigan,
Ann Arbor, MI, USA. From 2013 to 2014, he was a Post-Doctoral Fellow
with the Department of Materials and Interfaces, Faculty of Chemistry,
Weizmann Institute of Science, Rehovot, Israel. He is currently the leader of
the NEMS/MEMS and Nanomaterials Laboratory, Department of Mechanical
Engineering, Faculty Engineering Sciences, Ben-Gurion University of the
Negev, Beer-Sheva, Israel.