micromachines

Article
Piezoelectric MEMS Resonators for Cigarette
Particle Detection
Javier Toledo 1, * , Víctor Ruiz-Díez 1 , Maik Bertke 2 , Hutomo Suryo Wasisto 2 ,
Erwin Peiner 2 and José Luis Sánchez-Rojas 1
1 Microsystems, Actuators and Sensors Group, Universidad de Castilla-La Mancha, 13071 Ciudad Real, Spain;
victor.ruiz@uclm.es (V.R.-D.); joseluis.saldavero@uclm.es (J.L.S.-R.)
2 Institute of Semiconductor Technology (IHT), Technische Universität Braunschweig, Hans-Sommer-Straße
66, 38106 Braunschweig, Germany and Laboratory for Emerging Nanometrology (LENA), Langer Kamp 6a,
38106 Braunschweig, Germany; m.bertke@tu-braunschweig.de (M.B.);
h.wasisto@tu-braunschweig.de (H.S.W.); e.peiner@tu-braunschweig.de (E.P.)
* Correspondence: javier.toledo.serrano@gmail.com; Tel.: +34-926-295-300 (ext. 96667)




Received: 29 January 2019; Accepted: 19 February 2019; Published: 21 February 2019


Abstract: In this work, we demonstrate the potential of a piezoelectric resonator for developing
a low-cost sensor system to detect microscopic particles in real-time, which can be present in
a wide variety of environments and workplaces. The sensor working principle is based on the
resonance frequency shift caused by particles collected on the resonator surface. To test the sensor
sensitivity obtained from mass-loading effects, an Aluminum Nitride-based piezoelectric resonator
was exposed to cigarette particles in a sealed chamber. In order to determine the resonance parameters
of interest, an interface circuit was implemented and included within both open-loop and closed-loop
schemes for comparison. The system was capable of tracking the resonance frequency with a mass
sensitivity of 8.8 Hz/ng. Although the tests shown here were proven by collecting particles from
a cigarette, the results obtained in this application may have interest and can be extended towards
other applications, such as monitoring of nanoparticles in a workplace environment.

Keywords: microelectromechanical systems (MEMS); piezoelectric; aluminum nitride (AlN); low-cost

circuit; phase-locked loop; particle

1. Introduction
Microscopic particles are present in many environments, e.g., the aerospace, healthcare or
pharmaceutical industries, and workplaces. For this reason, many studies have been reported about
the adverse effects to human health due to their small size and the potential to cause respiratory
diseases [1–3]. Therefore, there is an increasing need to detect and control the concentration of
these particles in multiple contexts, motivating the development of a low-cost system capable
of detecting these particles in real-time. Several research groups established various types of
micro-/nanoelectromechanical systems (M/NEMS) as mass-sensitive sensors for this purpose [4–7].
The detection mechanisms and elements of the sensing systems have been varied, e.g., direct optical
investigation inside a scanning electron microscope for vertical nanowire resonators [8], square full
piezoresistive Wheatstone bridge for out-of-plane cantilevers [9], U-shape piezoresistive Wheatstone
bridge for in-plane electrothermal cantilevers [10], and thin piezoelectric films for bulk acoustic
devices [11,12].
Sampling of particulate matter for gravimetric detection usually requires a particle collector stage,
e.g., an impactor [13,14], a thermophoretic [11] or electrostatic sampler [4,8,9], an adhesive layer [15],
etc. Basically, that also applies to cigarette smoke particles, which were collected on a silicon cantilever

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cantilever resonator
resonator using using thermophoresis
thermophoresis [11], [13,14],
[11], an impactor an impactor [13,14], or an
or an electrostatic electrostatic
field fieldsmoke
[16]. However, [16].
However, smoke
particulates particulates
could be sampled could be sampled
without without
additional additional
measures measures
for particle for particle
collection, whichcollection,
was not
which was not observed so far
observed so far for other aerosols.for other aerosols.
InInthis
thiswork,
work,the
thesensor
sensorworking
workingprinciple
principleisisbased
basedon onthe
theresonance
resonancefrequency
frequencyshift
shiftinduced
inducedby by
collected
collectedparticles
particlesonon
a piezoelectric
a piezoelectricresonator surface
resonator [4,16].
surface For For
[4,16]. evaluating the sensor
evaluating sensitivity,
the sensor the
sensitivity,
resonator device
the resonator waswas
device exposed to cigarette
exposed particles
to cigarette in ainsealed
particles a sealedchamber,
chamber,ininwhich
whichthe
themass-loading
mass-loading
effect could subsequently be proven and analyzed.
effect could subsequently be proven and analyzed.

2.2.Materials
Materialsand
andsetup
Setup
For
Forthis
thisapplication,
application,an analuminum
aluminumnitride nitride(AlN)
(AlN)based
basedpiezoelectric
piezoelectricresonator
resonatorwas wasdesigned,
designed,
fabricated
fabricatedand and optimized for for aahigh-order
high-orderbending
bending mode.
mode. It isIt well
is well
knownknownthat that increasing
increasing modemodeorder,
order, the increase in Q-factor and resonance frequency as well as the decrease
the increase in Q-factor and resonance frequency as well as the decrease in effective mass improve the in effective mass
improve the mass
mass sensitivity of sensitivity
the resonator of [17,18].
the resonator
On the [17,18]. On the
other hand, lower other hand, lower
frequencies allowfrequencies allow
easier and cheaper
easier and designs
electronic cheaper for electronic
the signaldesigns for the signal
conditioning. In ourconditioning. In our case, amplifier
case, the instrumentation the instrumentation
shows a flat
amplifier
responseshows a flatcurve
in the gain response
up toinapproximately
the gain curve10up MHzto approximately
with a phase shift 10 MHz with aabove
appearing phase1 shift
MHz
appearing
that affectsabove 1 MHz that
the resolution affects
of the the resolution
system. Taking thisoflimitation
the system. intoTaking thiswe
account, limitation
chose the into account,
fourth order
we chose shaped
roof-tile the fourth order roof-tile
vibration mode near shaped vibration
1 MHz. mode near
This features five1nodal
MHz.linesThis in
features five nodal
one direction andlines
zero
innodal
onelines
direction and zero nodal
in the perpendicular lines Considering
direction. in the perpendicular direction. [19],
Leissa´s nomenclature Considering
the vibration Leissa´s
mode
nomenclature
is named as 05-mode[19], the [20].
vibration mode is named as 05-mode [20].
For
For an efficient excitationofofhigher
an efficient excitation higherorderordervibration
vibrationmodes,
modes,an anappropriate
appropriateelectrode
electrodelayout
layoutisis
required
requiredso sothat
thatthe
thetarget
targetmode
modeisisoptimally
optimallyexcited
excitedand
andsensed.
sensed.InInparticular,
particular,roof
rooftile-shaped
tile-shapedmodesmodes
are
areoptimally
optimallyactuated
actuatedusing
using a stripped
a stripped electrode
electrodedesign [12,21],
design [12,21],whichwhichallows a two-port
allows a two-port scheme. In
scheme.
order to prevent excessive damping associated with the substrate, the anchoring
In order to prevent excessive damping associated with the substrate, the anchoring of the plates to the of the plates to the
substrate
substrateframe
framewas was carefully
carefully designed
designed to reduce
reduce the
the energy
energydissipation.
dissipation.Beam Beamanchors
anchorswere wereplaced
placedat
atthe
thesame
same position as the nodes for a 05-mode, and their resonance frequency
position as the nodes for a 05-mode, and their resonance frequency was also coincident with was also coincident
with
that that oftarget
of the the target
mode. mode.
One
Onemoremoreaspect
aspecttotoconsider
considerininthe thedevice
devicedesign
designisisthe
themagnitude
magnitudeofofthe thearea
areaexposed
exposedtotothe the
particles. For this particular vibration mode, the resonance frequency is
particles. For this particular vibration mode, the resonance frequency is determined by the width determined by the width of
the anchored
of the anchored side.side.
The length alongalong
The length the nodal lines lines
the nodal is chosen to have
is chosen to both
have good
both signal to noise
good signal to ratio
noise
[22] and
ratio [22]a and
sensitive area much
a sensitive larger larger
area much than thethanparticles to be detected,
the particles to avoid
to be detected, edge effects.
to avoid The
edge effects.
fabricated
The fabricated resonator and its considered modal shape measured by a laser Doppler vibrometerare
resonator and its considered modal shape measured by a laser Doppler vibrometer are
shown
shownininFigures 1a and
Figure 1a,b, 1b, respectively.
respectively. The resonator
The resonator has a length
has a length of l =µm,
of l = 3000 3000 μm, a of
a width width of wµm
w = 900 =
900 μm and a thickness
and a thickness of t = 10 µm. of t = 10 μm.

Figure
Figure1.1.(a)
(a)Top-view
Top-viewmicrograph
micrographof ofthe
theresonator
resonator (3000
(3000 μm
µm ××900
900μm
µm××1010μm)
µm)and
andcompensation
compensation
device
devicein
in aa dual in-line
in-linepackage.
package.(b)
(b)Modal
Modal shape
shape measured
measured with
with a laser
a laser Doppler
Doppler vibrometer
vibrometer (05-
(05-mode).
mode).
The top metallization has four striped electrodes that allow a selective excitation of the vibration
modesTheand
topact as a filter forhas
metallization higher
fourmodes
striped[23]. The resonator
electrodes is excited
that allow by anexcitation
a selective anti-parallel connection
of the vibrationof
the electrodes
modes (+−
and act as −) tofor
a +filter obtain themodes
higher desired modal
[23]. Thevibrations.
resonator isInexcited
this case,
bytwo top electrodes
an anti-parallel connected
connection
ofinthe
parallel (+) were
electrodes usedtoasobtain
(+−+−) actuation ports and
the desired the other
modal two (−In
vibrations. ) asthis
sensing
case, ports (see electrodes
two top Figure 1b).
connected in parallel (+) were used as actuation ports and the other two (−) as sensing ports (see
Figure 1b). The structure is anchored with five supports in the nodal lines to resemble a free plate
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The structure is anchored with five supports in the nodal lines to resemble a free plate condition.
Subsequently, this leads to
condition. Subsequently, thisanleads
increased
to an piezoelectric
increased piezoelectricresponse compared to a singletoside
response compared clamped
a single side
cantilever structure with the same geometry and quality factor
clamped cantilever structure with the same geometry and quality factor [24]. The fabrication of the [24]. The fabrication of the micro-plate
resonator
micro-plate was carried out
resonator wasby MEMSCAP
carried out by(Durham,
MEMSCAP NC, USA), following
(Durham, NC, USA), thefollowing
PiezoMUMPs process [25]:
the PiezoMUMPs
aprocess
silicon[25]:on insulator (SOI) wafer with 10 µm-thick device layer
a silicon on insulator (SOI) wafer with 10 μm-thick device layer was covered with was covered with a 500 nm-thick
a 500
aluminum
nm-thick aluminumnitride (AlN) piezoelectric
nitride film. The film.
(AlN) piezoelectric silicon Thewas doped
silicon wasto doped
serve astoboth servebottom
as both electrode
bottom
and structural
electrode layer. As alayer.
and structural top electrode,
As a top aelectrode,
layer of aluminum
a layer of (1 µm) was (1
aluminum deposited
μm) wasatdeposited
the final device
at the
processing step.
final device processing step.
The
The values
values of the resonant
of the resonant parameters
parameters (i.e., (i.e., resonance
resonance frequencyfrequency (f(frr)) and
and quality
quality factor
factor (Q-factor)),
(Q-factor)),
were registered in air before the deposition of cigarette particles,
were registered in air before the deposition of cigarette particles, obtaining values of 1108 kHz obtaining values of 1108 kHz and and
185,
respectively.
185, respectively. For this Forwork,
this only
work,one device
only one wasdeviceused, wasbutused,
other butdevices
other from the same
devices fromproduction
the same
batch were characterized in terms of f r and Q-factor. Structures
production batch were characterized in terms of fr and Q-factor. Structures with the same with the same nominal dimensions
nominal
showed values of 1108 ± 2 kHz and 189 ± 10 for f r and
dimensions showed values of 1108 ± 2 kHz and 189 ± 10 for fr and Q-factor, respectively. Q-factor, respectively.
In this work,
In this work, no nosystem
systemhas hasbeen beenimplemented
implementedregarding regarding thethe sampling
sampling of of cigarette
cigarette particles
particles on
on the resonator surface [5]. The lack of additional sampling
the resonator surface [5]. The lack of additional sampling requirements is an advantage of requirements is an advantage of our
our
approach. However,after
approach. However, afterconducting
conductingseveral severalexperiments,
experiments, it was
it was observed
observed thatthat despite
despite removing
removing the
the
cigarette particles with N2, the initial value of the resonance frequency was shifted. This occurs
cigarette particles with N 2 , the initial value of the resonance frequency was shifted. This occurs
because
because the the ash
ash particles
particles coming
coming from from the the cigarette
cigarette can can bebe easily
easily cleaned
cleaned with with air air or
or NN22.. However,
However,
other
other types
types of particles exist
of particles exist such
such as as nicotine
nicotine or or tar
tar (tobacco
(tobacco residue)
residue) that
that may
may adhere
adhere to to the
the resonator
resonator
surface. To avoid this problem, a cleaning process with isopropanol
surface. To avoid this problem, a cleaning process with isopropanol was implemented after different was implemented after different
experiments.
experiments. In In addition,
addition, the the resonator
resonator chip chip could
could be be cleaned
cleaned with with isopropanol
isopropanol without without needing
needing to to
be removed before from its package. This is a clear advantage
be removed before from its package. This is a clear advantage over approaches where the resonant over approaches where the resonant
device
device isisconsidered
consideredtotobebe disposable
disposable and, thus,
and, has to
thus, hasbetoreplaced beforebefore
be replaced a decrease of particle
a decrease capture
of particle
efficiency is detected
capture efficiency [15].
is detected [15].
The
The resonant parameters change
resonant parameters change due due to to external
external environmental
environmental influences
influences on on the
the device
device andand
need to be determined in real-time. The detection of these parameters
need to be determined in real-time. The detection of these parameters can be performed using several can be performed using several
methods
methods [4,26,27].
[4,26,27]. The Thereal-time
real-timemonitoring
monitoringofofthe the resonant
resonant parameters
parameters may maybe be
challenging
challenging duedueto the
to
low-quality factors and parasitic effects present in the resonator
the low-quality factors and parasitic effects present in the resonator [12,28]. For this reason, an [12,28]. For this reason, an interface
circuit
interface based on resonators
circuit in two-port in
based on resonators configuration involving a parasitic
two-port configuration involving compensation device and an
a parasitic compensation
instrumentation
device and an instrumentation amplifier was used to cancel the parasitic effects (see our
amplifier was used to cancel the parasitic effects (see Figure 2). However, results
Figure 2).
show that a capacitive crosstalk across the actuation and sensing
However, our results show that a capacitive crosstalk across the actuation and sensing ports has a ports has a significant contribution
to the output
significant current. Totominimize
contribution the outputthis parasitic
current. component,
To minimize thisaparasitic
compensationcomponent, (dummy) device was
a compensation
introduced [23]. This additional device duplicates the structure
(dummy) device was introduced [23]. This additional device duplicates the structure of the resonator, of the resonator, being basically an
exact copy of the plate resonator, unreleased to prevent its vibration.
being basically an exact copy of the plate resonator, unreleased to prevent its vibration. As it can be As it can be observed in Figure 3,
the application
observed in Figureof the3,interface circuit results
the application of theininterface
a clear resonance, with in
circuit results low baseline
a clear and the necessary
resonance, with low
phase to meet the Barkhausen criterion for oscillation.
baseline and the necessary phase to meet the Barkhausen criterion for oscillation.

Figure 2.
2. Schematic of interface
Schematic circuit
of interface to measure
circuit the 05-mode
to measure response
the 05-mode by cancelling
response the parasitic
by cancelling the
capacitance.
parasitic capacitance.
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Figure 3.3. Open

Open loop
loopresponse
responseofofthe
theinterface
interfacecircuit forfor
circuit thethe
05-mode.
05-mode.Gain-phase
Gain-phase before represents
before the
represents
initial statestate
the initial of the resonator
of the in air,
resonator andand
in air, gain-phase
gain-phaseafter indicates
after thethe
indicates final state
final after
state thethe
after deposition of
deposition
cigarette particles.
of cigarette particles.

In
In addition,
addition, aa closed-loop circuit, based
closed-loop circuit, based on on the
the phase-locked
phase-locked loop loop (PLL)
(PLL) integrated
integrated circuit
circuit
74HCT4046
74HCT4046 [29], [29], is
is implemented
implemented for for tracking
tracking the the resonant
resonant parameters
parameters of of the
the resonator.
resonator. This This oscillator
oscillator
circuit
circuit isis aafeedback
feedbacksystem
system composed
composed of of a phase
a phase comparator
comparator (PC2),(PC2), a low-pass
a low-pass filter (Filter
filter (Filter 1) and 1)a
and a voltage-controlled
voltage-controlled oscillatoroscillator
(VCO).(VCO).
Basically, Basically, this circuit
this circuit is a feedback
is a feedback loop whereloop the where VCO thecan
VCObe
can be automatically
automatically synchronized
synchronized with thewith signal thecoming
signal from
comingthe from the resonance
resonance of the piezoelectric
of the piezoelectric resonator
resonator [30,31]. Besides, as it can be seen in Figure 4, the output
[30,31]. Besides, as it can be seen in Figure 4, the output signal of the VCO (fosc) was signal of the VCO (f osc ) was adapted
adapted with a
with a low-pass
low-pass filter 2)
filter (filter (filter
since2)thesince
VCO thegenerates
VCO generates a digital
a digital signal.signal.
In this In thisthe
way, way, the excitation
excitation of the
of the resonator is carried out with a filtered sinusoidal signal obtaining
resonator is carried out with a filtered sinusoidal signal obtaining a higher stability of the oscillationa higher stability of the
oscillation frequency. This oscillator circuit allows us to obtain
frequency. This oscillator circuit allows us to obtain a reference signal (fref), whicha reference signal (f ref ), which controls
controls the
the frequency
frequency and and
phase phase
of the ofoscillator.
the oscillator.
In thisIncircuit,
this circuit, the feedback
the feedback error issignal
error signal a phase is alag,
phase lag,
instead
instead of a voltage or current as in conventional feedback systems. The
of a voltage or current as in conventional feedback systems. The self-correcting capability of this self-correcting capability of
this system
system allows allows
the the
PLLPLL to modify
to modify thethe oscillation
oscillation frequency
frequency asasa afunction
functionofofmassmass changes
changes on on the
the
resonator
resonator surface
surface duedue toto the
the addition
addition of of particles.
particles.

Figure 4.
Figure 4. Schematic of phase-locked
Schematic loop loop
of phase-locked (PLL)(PLL)
74HCT4046 oscillator
74HCT4046 circuit including
oscillator the interface
circuit including the
circuit. circuit.
interface
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Methods
3. Measurements and methods
To demonstrate the functionality of the system, the resonator is characterized with different
open-loop and
and closed-loop
closed-loopconfigurations
configurationsand
andexperimental
experimentalarrangements.
arrangements.Finally, thethe
Finally, added mass
added of
mass
thethe
of cigarette particles
cigarette on on
particles thethe
resonator surface
resonator is estimated.
surface is estimated.

3.1. Open-Loop
3.1. Open-Loop Measurements
Measurements
Initially, the
Initially, the05-mode
05-mode waswas
analyzed withwith
analyzed an open-loop technique
an open-loop based onbased
technique a USBondataa acquisition
USB data
board, Digilent instrument Analog Discovery 2 (Digilent Inc., Pullman, WA, USA)
acquisition board, Digilent instrument Analog Discovery 2 (Digilent Inc., Pullman, WA, USA) [32], [32], capable of
performing sweep frequency measurements. This instrument is connected to a PC
capable of performing sweep frequency measurements. This instrument is connected to a PC in order in order to calculate
f r and
to Q-factor
calculate of the
fr and resonator
Q-factor since
of the these parameters
resonator since thesehave a large influence
parameters on the
have a large sensitivity
influence on and
the
efficiency of the mass concentration sensing principle. A schematic of the setup along
sensitivity and efficiency of the mass concentration sensing principle. A schematic of the setup alongwith the interface
circuit
with theisinterface
presented in Figure
circuit 5. The in
is presented sensor
Figureis 5.
separated
The sensorbyisa separated
distance ofby10 cm fromofthe
a distance 10 cigarette.
cm from
Thiscigarette.
the prevents larger particles from
This prevents largerdepositing directly
particles from on the resonator
depositing directlysurface.
on the In addition,surface.
resonator the sensor
In
is located on the same printed circuit board (PCB) next to the interface circuit.
addition, the sensor is located on the same printed circuit board (PCB) next to the interface circuit.

Figure 5. Schematic
Schematic of the open-loop setup with the Digilent instrument.

In the first step, the performance of the resonator was evaluated by collecting cigarette particles
on the surface resonator for 15 minutes and subsequently subsequently measuring
measuring the the frequency
frequency shiftshift produced.
produced.
As it can
can be
beobserved
observedininFigure
Figure3,3,a afrequency
frequency shift
shift of of around
around 10 10
kHzkHzwaswas detected
detected after
after sampling
sampling the
the particles. Nevertheless, a phase shift −15is is◦
particles. Nevertheless, a phase shift of of around−15°
around observeddue
observed duetotodifferences
differences between
between the
dummy and resonator, and the bandwidth limitation of the the instrumentation
instrumentation amplifier.
amplifier. However,
However, this
resonance curve is adequate for the later implementation of the oscillator oscillator circuit.
circuit.
Once the behaviors of the resonator and electronic system were tested, two similar experiments
for the detection of cigarette particles were performed. The main objective was to check the deposition deposition
rate of
of the
thecigarette
cigaretteparticles
particlesand
andthe
thereproducibility
reproducibility of the measurements. In this case,
of the measurements. In this case, we carried we carried
out
aout a frequency
frequency sweep
sweep every
every minute.
minute. In In order
order totocalculate
calculatethe theresonant
resonant parameters,
parameters, the the measured
impedance spectrum
impedance spectrum was
was fitted
fitted to
to aa modified
modified Butterworth-Van-Dyke
Butterworth-Van-Dyke (BVD) (BVD) equivalent
equivalent circuit
circuit [33].
[33].
The frequency resolution measured of the resonator was 70 Hz, a rather high value compared with
other results [12,20], associated with the open-loop configuration and the commercial instrument
employed in the measurements.
In Figures 6 and 7, the open-loop measurements are displayed showing the evolution of the
resonant parameters with the deposition of cigarette particles. As As expected
expected from
from thethe previous
previous results,
results,
frrand Q-factordecreased
andQ-factor decreased over
over time
time due
due toto aa higher
higher concentration
concentration of of cigarette
cigarette particles on the surface
resonator. More
resonator. More deposited
depositedcigarette
cigaretteparticles
particlesresult
resultininhigher
higherfrequency
frequency shifts.
shifts.AsAsit can bebe
it can observed
observed in
Figures
in Figures6 and
6 and7, 7,
anan
almost
almost linear decrease
linear decreaseoccursoccursforforf rfrand
andQ-factor
Q-factor obtaining
obtaining aa decrease of around
−1 , respectively.
625 ±±88Hz/min
Hz/minand −0.55
and−0.55 ± 0.03
± 0.03 minmin
−1, respectively.
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Figure 6.
Figure 6. Open
6. Open loop
Open loop measurement
loop measurement showing
measurement showing the
showing the evolution
the evolution of
evolution of the resonant
of the resonant parameters
parameters with
with the
the
deposition of cigarette particles
cigarette particles
deposition of cigarette for
particles for 10
for 10 minutes.
10 minutes.
minutes.

Figure 7. Open
Figure 7.
7. Open loop
Open loop measurement
loop measurement showing
measurement showing the
showing the evolution
the evolution of the
evolution of the resonant
resonant parameters
parameters with
with the
the
deposition of cigarette
cigarette particles
particles for
for 15
15 minutes.
minutes.
deposition of cigarette particles for 15 minutes.

The
The slight
The slight linear
slight linear decrease
linear decrease of
decrease of Q(t)
of Q(t) observed
Q(t) observed in
observed in Figures
in Figures 666 and
Figures and 777 indicates
and indicates that
indicates that the
that the roof-tile-shaped
the roof-tile-shaped
roof-tile-shaped
vibration
vibration mode
mode is
is sensitive
sensitive to
to a
a damping
damping effect
effect by
by the
the deposited
deposited cigarette
cigarette particles.
particles. This
This effect
effect can
can bebe
vibration mode is sensitive to a damping effect by the deposited cigarette particles. This effect can be
explained
explained through
through Equation
Equation (1),
(1), which
which shows
shows that
that an
an increase
increase in
in Q-factor
Q-factor might
might be
be expected
expected with
with the
the
explained through Equation (1), which shows that an increase in Q-factor might be expected with the
added
added mass
massofofofthethecigarette
cigaretteparticles
particles (∆m(Δmcig )cig
assuming
) assuming a uniform
a uniformdeposition. [34]. [34].
deposition. However, their effect
However, their
added mass the cigarette particles (Δm cig) assuming a uniform deposition. [34]. However, their
in Q-factor
effect in may also
Q-factor maylead to lead
also an increased
to an viscous viscous
increased dampingdamping
(cdamp ), due
(𝑐 to),the
duepresence
to the of big particles
presence of big
effect in Q-factor may also lead to an increased viscous damping (𝑐 ), due to the presence of big
with irregular
particles with shape
with irregular [9] (see
irregular shape Figure
shape [9]
[9] (see12).
(see Figure
Figure 12). 12).
particles
∆mcig
q
1 + ∆𝑚 ∆𝑚
Q- f actor = 2π f can mcan 1 1+ + mcan
cdamp𝑚𝑚 (1)
(1)
(1)
𝑄 -factor =
𝑄-factor = 2𝜋𝑓 𝑚 2𝜋𝑓 𝑚
𝑐𝑐
where f can , mcan and cdamp are the resonator frequency before particle deposition, mass resonator and
where
viscous can, mcan and cdamp are the resonator frequency before particle deposition, mass resonator
ffcan
damping,
where , mcanrespectively.
and cdamp are the resonator frequency before particle deposition, mass resonator
and viscous
Regarding
and viscous damping, respectively.
the evolution
damping, of resonance frequency with time, assuming both constant concentration
respectively.
Regarding
of cigarette particles
Regarding the evolution
theinevolution
the ambientof ofairresonance
resonance
and constant frequency
adsorption
frequency with
rate of
with time, assuming
theseassuming
time, both
particles onboth constant
the resonator,
constant
concentration of
concentration of cigarette
cigarette particles
particles in in the
the ambient
ambient air air and
and constant
constant adsorption
adsorption raterate of
of these
these particles
particles
on the resonator, we can expect a constant decrease rate Δf r/Δt and thus a linear decrease of fr(t) as
on the resonator, we can expect a constant decrease rate Δfr/Δt and thus a linear decrease of fr(t) as
confirmed by
confirmed by ourour experiments
experiments in in Figures
Figures 66 and and 7. 7. The
The added
added mass
mass will
will be
be estimated
estimated in in section
section 3.3.
3.3.
Micromachines 2019, 10, 145 7 of 13

we can expect a constant decrease rate ∆f r /∆t and thus a linear decrease of f r (t) as confirmed by our
experiments in Figures 6 and 7. The added mass will be estimated in Section 3.3.

3.2. Closed-Loop Measurements

In the previous section, we could check that the open-loop technique presents a poor frequency
resolution. In addition, this technique requires a long measurement time, limiting the potential
application 2019,
Micromachines in a real-time
10, x monitoring system. For this reason, a low-cost PLL-based oscillator circuit, 7 of 13
utilizing the previously described 74HCT4046, was developed.
3.2. Closed-Loop Measurements
The implementation of an oscillator is challenging due to the hydrodynamic loading (damping in
air) and parasitic effects
In the previous section, ofwethecould
resonator, which
check that the increase
open-loopfortechnique
larger surfaces.
presents aFor
poorthis reason,
frequency
the previously described interface circuit with dummy compensation was also included
resolution. In addition, this technique requires a long measurement time, limiting the potential in the system.
In this setup,
application inthe PLL circuit
a real-time was combined
monitoring system.with
Forthe
thisresonator
reason, a and the previous
low-cost PLL-basedinterface circuit
oscillator as a
circuit,
closed-loop oscillator system as shown in Figure 8.
utilizing the previously described 74HCT4046, was developed.

Figure 8. Schematic of the closed-loop setup with the PLL 74HCT4046.

In order
The to obtain theof
implementation resonant parameters,
an oscillator it was necessary
is challenging due to the to hydrodynamic
perform a calibration loading process
(damping [35].
In air)
in this and
process, the oscillator
parasitic effects ofcircuit outputs, which
the resonator, oscillation frequency
increase (f oscsurfaces.
for larger ), and theFor
circuit
thisoutput
reason,gainthe
(G osc ) were described
previously transformed into the
interface mechanical
circuit with dummymagnitudes was also fincluded
of the resonator,
compensation r and Q-factor, using a
in the system.
resonator
In model
this setup, [36]. circuit
the PLL In this was
case,combined
the commercial
with the instrument
resonator wasand able to obtaininterface
the previous the circuit outputs,
circuit as a
fclosed-loop
osc and G , with a rate of 5 samples/s
oscoscillator system as shown in Figure 8.obtaining a better frequency resolution of 1 Hz. To test the
system performance,
In order to obtaintwo different parameters,
the resonant experimentsitwere carried out
was necessary towith
perform the closed-loop
a calibrationsetup.
processIn[35].
the
first
In experiment,
this process, the particles were
oscillator collected
circuit as inoscillation
outputs, the previous section obtaining
frequency (fosc), and athedecrease
circuit rate f r of
for gain
output
around
(G 621 transformed
osc) were Hz/min (see into Figure the9).mechanical magnitudes of the resonator, fr and Q-factor, using a
resonatorIn themodel
second[36].experiment, the sensitivity
In this case, and response
the commercial of thewas
instrument system
ablewere further
to obtain thechecked. In order
circuit outputs,
fto
osc do
andthat,
Goscwe
, withintroduced
a rate of an additionalobtaining
5 samples/s cigarette ainbetter
the chamber
frequency andresolution
opened and of 1closed
Hz. Toit test
several
the
times, toperformance,
system assess the response of the experiments
two different system. As itwerecan be observed
carried in Figure
out with 10, several setup.
the closed-loop peaks In in the
resonance
first curves particles
experiment, were detected as a consequence
were collected as in theof this. Besides,
previous sectionwe could check
obtaining that therate
a decrease deposition
for fr of
of particles
around 621 was
Hz/min higher,
(seewith a decrease
Figure 9). rate for f r of around 1690 Hz/min, when two cigarettes were
introduced at the same
In the second time in the
experiment, thesealed chamber.
sensitivity and response of the system were further checked. In
order to do that, we introduced an additional cigarette in the chamber and opened and closed it
several times, to assess the response of the system. As it can be observed in Figure 10, several peaks
in the resonance curves were detected as a consequence of this. Besides, we could check that the
deposition of particles was higher, with a decrease rate for fr of around 1690 Hz/min, when two
cigarettes were introduced at the same time in the sealed chamber.
The open-loop measurements displayed in Figures 6 and 7 as well as the closed-loop
measurements in Figure 9, which were carried out with the smoke of one cigarette in the chamber,
Micromachines 2019, 10, x 8 of 13
Micromachines 2019, 10, x 8 of 13

smoke from2019,
Micromachines the10,
resonator
145 by evaporation, which is reasonable owing to the considerable amount
8 of 13
smoke from the resonator by evaporation, which is reasonable owing to the considerable amount
semivolatile components in cigarette smoke, e.g., nicotine and water [37].
semivolatile components in cigarette smoke, e.g., nicotine and water [37].

Figure 9.
9. Closed
Closed loop
loop measurement
measurement showing
showing the
the evolution
evolution of the resonant parameters with the
Figure 9. Closed loop measurement showing the evolution of the resonant parameters with the
from one
deposition of particles from one cigarette.
cigarette.
deposition of particles from one cigarette.

Figure 10. Closed loop measurement showing the evolution of the resonant parameters with the
Figure 10. Closed
10. Closed loop measurement
measurement showing
showing the evolution of the resonant parameters with the
deposition of particles from two cigarettes.
from two
deposition of particles from two cigarettes.
cigarettes.
Figures 11 and 12 show sensor top-view images obtained with a scanning electron microscope
The open-loop
Figures 11 and 12measurements
show sensor displayed
top-view in Figures
images obtained6 with
and a7 scanning
as well electron
as the closed-loop
microscope
(SEM). The SEM images depict the resonator covered by particles of different sizes and shapes. The
measurements
(SEM). The SEM inimages
Figure depict
9, which
thewere carried
resonator out with
covered by the smoke
particles ofof one cigarette
different in the
sizes and chamber,
shapes. The
previous measurements show that these particles can be detected in real-time with a low-cost
show almost
previous monotonic decrease
measurements show that f r andparticles
of these Q-factor can
withbetime. Fluctuations
detected of both
in real-time f r (t)
with a and Q(t)
low-cost
oscillator circuit.
about the fitted
oscillator circuit.straight lines are visible in Figure 9, and Figure 10 shows even slight increases of
both parameters caused by opening of the chamber and the corresponding concentration decrease of
cigarette particles inside the chamber. We attribute this effect to a transient loss of deposited cigarette
smoke from the resonator by evaporation, which is reasonable owing to the considerable amount
semivolatile components in cigarette smoke, e.g., nicotine and water [37].
Figures 11 and 12 show sensor top-view images obtained with a scanning electron microscope
(SEM). The SEM images depict the resonator covered by particles of different sizes and shapes.
The previous measurements show that these particles can be detected in real-time with a low-cost
oscillator circuit.
Micromachines 2019, 10, 145 9 of 13
Micromachines 2019, 10, x 9 of 13

Figure 11. Micrograph

Micrograph ofof the
the 05-mode
05-mode resonator
resonator and
and the dummy device with scanning electron
microscope (SEM) after the deposition of cigarette
cigarette particles.
particles.

Figure
Figure 12.
12.Micrographs of different
Micrographs cigarette
of different particlesparticles
cigarette depositeddeposited
on the surfaces
on theof surfaces
a piezoelectric
of a
resonator.
piezoelectric resonator.
Micromachines 2019, 10, 145 10 of 13

3.3. Estimation of Added Mass

Once the performance of the resonator was tested with different open-loop and closed-loop
techniques, the mass of the deposited cigarette particles, ∆mcig , can be estimated through
Equation (2) [16,38]:
2mcan
∆mcig ' ∆ f cig (2)
f can
where ∆f cig , f can , mcan are the frequency shift after particle deposition, resonator frequency before
particle deposition, and mass, respectively.
This expression is under the assumption that the spring constant of the resonator is maintained
and that the deposition of particles is uniform on the surfaces. The resonator used in this work has
a mass of mcan = 62.91 µg and a resonance frequency in air of f can = 1108 kHz. The added mass was
estimated for the second open loop measurement presented in Figure 7. In that case, a frequency shift
(∆f cig ) of around 10 kHz was detected after collecting particles for 15 minutes, obtaining a value of
∆mcig = 1.14 µg. Moreover, the mass-loading sensitivity of the sensor (∆f cig /∆mcig ) was calculated
obtaining a value of 8.8 Hz/ng. This sensitivity value is similar to that reported by Wasisto et al. of
0.15 Hz/ng for a cantilever sensor of smaller dimensions with a lower resonance frequency [38].
This sensitivity was obtained using a USB data acquisition board (Digilent instrument, Digilent
Inc., Pullman, WA, USA) and the closed-loop technique with a frequency resolution of 1 Hz.
A frequency resolution of around 8 mHz could be achieved with the same device but using a higher-cost
instrument such as a lock-in amplifier [39]. With these two values for the resolution in the tracking of
resonance frequency and the sensitivity given above, the limit of detection can be 114 pg or 1 pg for
the two measurement configurations, respectively. The sensitivity of the resonator was also estimated
and compared taking into consideration the surface of the resonator, obtaining a sensitivity ratio of
21.4 µm2 /ng. This value is also similar to that reported by Wasisto et al. of 8.54 µm2 /ng [4].

3.4. Discussion
M/NEMS-based gravimetric sensors for cigarette smoke detection have been already reported,
with different strength and weaknesses. As it can be seen in Table 1, mass sensitivity up to several
tens of Hz/pg and resolution of 29.8 fg have been stated, which are clearly better than the values of
8.8 Hz/ng and 114 pg, respectively, obtained in this work. However, our device has a larger surface
compared to the size of the particles. In this way, edge effects can be neglected since the particles are
uniformly distributed on the resonator surface.

Table 1. M/NEMS-based resonators for gravimetric cigarette smoke detection.

M/NEMS Particle PLL for Frequency Mass Mass

Reference
Resonator Sampler Tracking Sensitivity Resolution
FBAR 1 thermophoretic integrated not given 2 µg/m3 [11]
TPR 2 impactor not given 42 Hz/pg not given [13]
TPR 2 impactor external 1.9 Hz/pg 29.8 fg [14]
PCR-NWA 3 no no 20 Hz/ng 50–100 pg [40]
PCR 4 electrostatic integrated 12 Hz/ng 76.2 pg [16]
PPR 5 no integrated 8.8 Hz/ng 114 pg This work
1 FBAR: film bulk acoustic resonator. 2 TPR: thermal-piezoresistive resonator. 3 PCR-NWA: piezoresistive cantilever
resonator with nanowire array. 4 PCR: piezoresistive cantilever resonator. 5 PPR: piezoelectric plate resonator.

Besides, the present approach has the advantage that no particle sampler is required due to the
large surface of the sensor and frequency tracking is performed using an integrated, low-cost PLL
circuit. Furthermore, in our case we can clean the resonator chip without needing to remove it from
its package using N2 and isopropanol. These issues, although not stressed in the other studies, are
Micromachines 2019, 10, 145 11 of 13

directly related to the planned use of such sensors in portable applications, i.e. monitoring of personal
aerosol exposure.

4. Conclusions
In conclusion, the development of a closed-loop circuit setup based on a piezoelectric micro-plate
resonator and the integrated circuit 74HCT4046 has been demonstrated. The system is capable
of tracking the resonance frequency and quality factor of the device, oscillating in a high order
vibrational mode (05-mode), with a sensitivity of 8.8 Hz/ng and a resolution of 114 pg. In this case,
the mass-loading effect tests were proven by collecting particles from a cigarette. Nevertheless,
the results obtained in this application may have potential applications for the detection of
nanoparticles in a workplace environment.

Author Contributions: Investigation, J.T.; Project administration, J.L.S.-R.; Supervision, V.R.-D., M.B., H.S.W., E.P.
and J.L.S.-R.; Validation, J.T.; Writing—original draft, J.T.; Writing—review & editing, V.R.-D., M.B., H.S.W., E.P.
and J.L.S.-R.
Funding: This work was supported by the Spanish Ministerio de Economía y Competitividad and FEDER
project TEC2015-67470-P. Junta de Comunidades de Castilla-La Mancha project SBPLY/17/180501/000139 and
through grant PEII-2014-010-P. Javier Toledo acknowledges financial support from the FPI-BES-2013-063743 grant.
Hutomo Suryo Wasisto thanks the Lower Saxony Ministry for Science and Culture (N-MWK) for funding of
LENA-OptoSense group. Maik Bertke acknowledges support from Niedersächsisches Vorab, Germany, through
the Quantum and Nanometrology (QUANOMET) initiative within the project of NP 2-2.
Conflicts of Interest: The authors declare no conflict of interest. The funders had no role in the design of the
study; in the collection, analyses, or interpretation of data; in the writing of the manuscript, or in the decision to
publish the results.

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