Sensors and Actuators A 298 (2019) 111607

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Sensors and Actuators A: Physical

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Wearable transcutaneous oxygen sensor for health monitoring

Chang-Jin Lim, Jin-Woo Park ∗
Department of Materials Science and Engineering, Yonsei University, 50 Yonsei-ro, Seodaemun-gu, Seoul 03722, Republic of Korea

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

Article history: We present a wearable bandage-like photoluminescence (PL)-based transcutaneous oxygen (tcpO2 ) sen-
Received 15 July 2019 sor consisting of a photoluminescent oxygen (O2 )-sensing film, a polyvinylidene chloride (PVDC) film
Received in revised form 3 September 2019 as an encapsulation layer, an indium tin oxide (ITO) thin-film heater, an array of micro-light-emitting
Accepted 6 September 2019
diodes (␮-LED) as a light source, red cellophane paper as an optical filter, an organic photodiode (OPD)
Available online 7 September 2019
as a PL detector, and an optical isolation layer. All the components of the tcpO2 sensor were designed
to be flexible and thus can be attached anywhere on the curved skin of the human body. The PVDC film
Keywords:
with excellent O2 barrier properties and visible light transmittance was a significant additional compo-
Transcutaneous oxygen monitoring
Luminescent oxygen sensing
nent of the wearable sensor that improved the sensitivity of the photoluminescent O2 -sensing film by
Wearable sensors minimizing the PL quenching effects of ambient atmospheric O2 . Furthermore, the ITO thin-film heater
Micro light-emitting diodes increases the skin temperature, changing the structure of the stratum corneum and allowing O2 to more
Organic photodiodes effectively diffuse from the skin toward the tcpO2 sensor. Therefore, the thin-film heater allows the accu-
rate measurement of the tcpO2 variation from human skin to facilitate the determination of the severity
of O2 -deficiency related diseases in the tcpO2 range from 0 to 80 mmHg. The ␮-LED array embedded into
a polydimethylsiloxane (PDMS) film not only maintained its mechanical flexibility but also had stable
light emission performance under ambient air conditions, allowing tcpO2 measurements over several
cycles for as long as 60 min, which we could not previously achieve with ambient air-unstable flexible
organic light-emitting diodes (f-OLEDs). The effects of the heat from the ITO thin-film heater and the skin
color of the sensor user on the PL emitted by the sensing film and detected by the OPD were factored out
from the tcpO2 measurements by defining two correction coefficients. The performance of the wearable
tcpO2 sensor was tested using the leg elevation protocol to induce tcpO2 variation at the skin of the
ankles of test volunteers. According to the experimental results, the sensing performance of our wear-
able bandage-like PL-based tcpO2 sensor proved to be superior to that of a commercially available tcpO2
sensor, as our wearable PL-based tcpO2 sensor demonstrated faster response times to tcpO2 variation
and smaller measurement deviations between tcpO2 detection cycles.
© 2019 Elsevier B.V. All rights reserved.

1. Introduction disease, Burger’s disease, varicose veins, and cerebral cardiovascu-

Oxygen (O2 ) is an essential component in energy production
and tissue regeneration to maintain human life [1]. A lack of O2 in
the human body causes various problems in its functions and, in
severe instances, results in the development of diseases [2]. If the
blood vessels are narrowed or clogged and O2 delivery to the tissues
and organs is limited, severe diseases such as cerebral infarction,
myocardial infarction, and diabetic ulcers can occur in patients
[3,4]. In particular, peripheral vascular disease (PVD), caused by the
inability to transfer O2 throughout the whole body, especially the
arms and legs, affects diseases such as diabetic ulcers, Raynaud’s
∗ Corresponding author.
E-mail address: jwpark09@yonsei.ac.kr (J.-W. Park).
lar disease [5].
Many elderly are very prone to O2 transmission-related dis-
eases that, if left untreated, can lead to numbness, gangrene, limb
amputation, and even death [6]. In contrast, if the tissue oxygen
concentration ([O2 ]) can be accurately measured, early symptom
detection and increased surgical success rates are possible [7].
Many published works have shown that tissue O2 pressure can be
a symptom of a wide range of peripheral capillary diseases, such
as cerebral vascular and spinal diseases [8,9]. In addition, the prog-
nosis of vessel occlusion after organ transplants, such as free-flap
surgery, is very important. Hence, a precise method for continu-
ously measuring [O2 ] in real time over a large surface area has
become a significant issue in health care and medicine [10–12].
There are many conventional methods for measuring the [O2 ]
in the human body. Among these methods, the Clark electrode is

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2 C.-J. Lim and J.-W. Park / Sensors and Actuators A 298 (2019) 111607
the most extensively used for measuring [O2 ] through an electro-
chemical reaction. However, it is an invasive approach involving
the consumption of the analytes during measurements as well as
inflicting pain and suffering on the patient because of the need for
the electrode to be pierced into the skin [13]. Alternatively, oxime-
try is a noninvasive spectroscopy-based method, but it is an indirect
method for measuring the hemoglobin concentration at the earlobe
or finger of a patient rather than a direct measurement of the [O2 ]
at a specific and desired part of the human body [14]. The laser
Doppler method is also an indirect and expensive method for cal-
culating the [O2 ] from the blood flow rate, which is not necessarily
proportional to [O2 ], and requires skilled personnel to apply [15].
These limitations have led to studies suggesting measuring [O2 ]
directly from the skin or tissue surfaces of the human body. The
tcpO2 is the O2 partial pressure measured on the surface of the skin
or tissue [16]. Huch et al. reported that the tcpO2 measured at the
skin surface has a high correlation with the arterial partial O2 pres-
sure (PaO2 ) [17]. Thus, tcpO2 reflects the O2 supply to the tissue
and can be used to diagnose O2 deficiency-related diseases [18].
Additionally, luminescence-based sensing methods have also
been widely studied as a means of replacing the conventional [O2 ]
measurement methods discussed above [19]. Unlike conventional
point analysis approaches, luminescence-based sensor systems are
noninvasive and can be miniaturized because there is no restriction
on their shapes or sizes [20]. Luminescence-based sensing methods
generally consist of a sensing component containing a phosphores-
cent dye whose emission intensity differs depending on the [O2 ],
a light source for exciting the sensing dye, and a detector for mea-
suring the photoluminescent light emitted by the dye. The [O2 ]
measured using a luminescence-based sensor can be quantified
using the Stern-Volmer function:
I0
= 1 + KSV [O2 ]
I stability and reproducibility of the performance of our bandage-like
where I0 and I correspond to the photoluminescence (PL) intensi-
ties in the absence and presence of O2 , respectively [21]. KSV is the
Stern-Volmer constant, and [O2 ] is the concentration of O2 [21].
Meanwhile, interest in wearable optoelectronics including the
devices needed in the healthcare technology is gradually increas-
ing according to current market trend analysis. In particular, in the
case of sensors applied to the human body, they need to be in close
contact with the curved surface of the human body and requires
high flexibility to increase their detection accuracy [22]. Until now,
various research groups have been working on materials selection
and/or various sensor structures for realizing the potential of wear-
able devices. Nalwa et al., developed wearable electronics for such
as wearable sensors based on 2D materials including graphene and
molybdenum disulfide (MoS2 ) atomic layers [23,24]. On the other
hand, Pan et al., fabricated a triboelectric tactile sensor on a struc-
tural elastomeric substrate [25].
In our previous study, we developed a wearable bandage-like
PL-based O2 sensor applying Eq. (1) by integrating a flexible photo-
luminescent O2 -sensing film, a flexible organic light-emitting diode
(f-OLED), a flexible optical filter, and a flexible organic photodiode
(f-OPD) into a single platform [26]. As a result, it was confirmed
that the tcpO2 measured from the skin of a fingertip and lower arm
increased as pressure was applied using a cuff and then decreased
again after the pressure was released. This finding suggests that
the amount of O2 dissolved in the skin and tissues that diffused
is increased by the pressure applied by a cuff on the nearby blood
vessels [27]. In addition, our previous results measured on the fin-
gertip and lower arm showed a very similar tendency to the tcpO2
values measured using the PeriFlux 5000, a commercially available
tcpO2 sensor, with our bandage-like luminescence-based O2 sensor
having a 1.5 times faster response time [27].
Interestingly, the steady-state tcpO2 of healthy individuals that
we previously measured using our wearable bandage-like PL-based
O2 sensor was approximately 25 to 35 mmHg, which much lower
than the tcpO2 range from 50 to 80 mmHg expected from a healthy
person [28–31]. Based on published works by other groups, this dis-
crepancy was because the temperature of the O2 probe or sensor
plays a very important role in the tcpO2 measurement and because
most of the published experiments were carried out while keep-
ing the temperature of the tcpO2 probe at 44 to 45 ◦ C [32–37]. This
temperature dependence occurs because when the skin is heated,
there is sufficient arterialization [38]. Heating the skin increases
the diffusion of O2 through the corneal layer [39]. In addition, heat-
ing the skin also causes the capillary blood vessels to expand and
the flow of blood through the skin to increase. This increased blood
flow provides more O2 to the heated skin [38]. It was shown in other
published works that elevated skin temperature affected only the
diffusion of tcpO2 through the skin and did not affect the detec-
tion of PVDs, which are driven by the ineffectiveness of the human
body in providing O2 to different organs through blood circula-
tion [40,41]. However, excess heat can have detrimental effects on
OLED-based sensors such as our previously developed bandage-like
PL-based O2 sensor [42,43].
In this study, we fabricated a transparent indium tin oxide
(ITO) thin-film heater and integrated it into our bandage-like
PL-based O2 sensor to increase the skin temperature during its
usage such that the increase in the transdermal O2 partial pres-
sure can be controlled as needed; thus, the tcpO2 can be more
accurately measured. In addition, the f-OLEDs serving as the light
excitation component of the sensor were replaced with ambi-
ent air-stable micro-light-emitting diode (␮-LED) arrays that still
maintain mechanical flexibility and have a very narrow full width at
half maximum (FWHM) of their emission spectra, enabling excel-
lent PL excitation of the O2 -sensing film. Hence, the long-term
(1)
PL-based O2 sensor were properly evaluated.
In addition, we investigated the effects of heat on the multicom-
ponent PL sensor and suggested a correction factor for its effects
on the tcpO2 measurements. Considering the effect of skin color
on PL detection, the accuracy of the intensity-based photocurrent
measurements was improved by introducing simple correction
coefficients in the tcpO2 calculation to compensate for the effect of
the skin color and temperature. Finally, the bandage-like PL-based
O2 sensor was used to measure the tcpO2 variation in a human leg
positioned at varying elevations with respect to the body, and its
performance was compared with that of an existing commercially
available tcpO2 sensor.
2. Experimental procedures
2.1. -LED array fabrication and characterization
The fabrication processes of the O2 -sensing film and the organic
photodiode (OPD) are described in detail in our previous study
[44,45]. The typical phosphorescent material 2,3,7,8,12,13,17,18-
octaethyl-21H,23H-porphyrin, platinum(II) (PtOEP, purity ≥ 98%,
Sigma-Aldrich, USA) was the main component of the sensing film.
PtOEP was mixed with Titanium dioxide (TiO2 ) nanoparticles (NPs)
in polystyrene (PS) solution to prepare the O2 -sensing film. Liq-
uid polydimethylsiloxane (PDMS) was prepared by mixing the base
elastomer with a curing agent at a weight ratio of 10:1. The PDMS
mixture was then poured into a mold after the trapped air bubbles
were degassed from the mixture. A 2-by-2 ␮-LED array (␮-LED, FC-
2012WBY-460 G, Foshan NationStar Optoelectronics, CHINA) with
metal wires for external electrical power input was then embedded
into the liquid PDMS before curing the elastomer for 48 h under
 C.-J. Lim and J.-W. Park / Sensors and Actuators A 298 (2019) 111607
ambient air conditions. The ␮-LED array was then connected to
a 9 V battery together with an on/off switch. The electrolumines-
cence spectrum and brightness of the ␮-LED were measured using
a CS-2000 chromameter (KONICA MINOLTA, USA).
2.2. ITO thin-film heater fabrication and characterization
An ITO thin film was deposited on a 50 ␮m-thick polyimide
(PI) substrate using a DC magnetron sputtering system at a sput-
tering power of 50 W. The thickness and area of the ITO thin film
were 100 nm and 17 mm x 17 mm, respectively. After applying Ag
paste on two opposing edges of the ITO thin film, Cu tape was
then attached to the two opposing edges of the ITO thin films to
act as the electrodes for electrical power input from an external
power supply. The temperature of the heater was measured using
an infrared (IR) camera (NEC Avio InfRec R300, JAPAN) positioned
20 degrees from the normal line of the heater surface. The aver-
age electrical line resistance of the ITO thin film was obtained from
three specimens using a two-point probe. The optical transmittance
spectrum of the ITO thin-film heater was measured using a UV–vis
spectrophotometer (V-650, JASCO, JAPAN).
2.3. Structural integration of the wearable transcutaneous sensor
The multicomponent wearable bandage-like tcpO2 sensor
shown in Fig. 1 was composed of an O2 -sensing film, a
polyvinylidene chloride (PVDC) film (LWP490, ASAHIKASEI HOME
PRODUCTS, JAPAN) for eliminating the effect of ambient O2 , an ITO
thin-film heater to increase skin surface temperature, a ␮-LED array
as a light source, red cellophane as a red-light filter, an OPD as a PL
detector, and an optical isolation layer for blocking ambient light
from interfering with the signal processing. All the components of
the bandage-like tcpO2 sensor were structurally integrated using PI
tape. The photocurrent signal of the OPD was amplified by a pho-
todiode amplifier (PDA200C, Thorlabs, USA) and transferred to a
data acquisition (DAQ) module (USB-6353, National Instruments,
USA) connected to LabVIEW software (LabVIEW 2012 SP1, National
Instruments, USA).
2.4. Participants
Healthy adults without any clinical history of PVDs or diabetes
participated in the experiments using our bandage-like tcpO2 sen-
sor. A written document including the detailed descriptions of this
experimental procedure was thoroughly examined and accepted by
the participants. This study was conducted in accordance with the
Declaration of Helsinki and approved by the Institutional Review
Board (IRB) of Yonsei University (IRB number: 7001988-201902-
HR-520-03).
2.5. tcpO2 sensor measurements
Participants were kept in bed one at time during their test
participation in a laboratory where the room temperature was
maintained at 25 ◦ . Body hair was removed from the skin area of
the foot of the test subject where the tcpO2 sensors were attached.
The skin area was cleaned prior to the attachment of the sensors
by wiping it with ethanol-wetted wipes. A PeriFlux 5000 (with a
tcpO2 unit, PF5040, PERIMED Co., Ltd., SWEDEN) and our bandage-
like tcpO2 sensor were alternately used to measure the tcpO2 from
the foot of our test subject as the foot was elevated at a 60 degrees
angle for 8 min and subsequently laid down flat for another 8 min.
The foot elevation and subsequent relaxation were repeated thrice
to complete one session of tcpO2 sensor performance evaluation.
3
Prior to the proper tcpO2 sensor evaluation, all the signals from the
sensors were made to be stable for approximately 11 min.
3. Result and discussion
Fig. 1a and b show a schematic diagram of the wearable
bandage-like tcpO2 sensor together with its multiple component
devices. As shown in Fig. 1a, the wearable tcpO2 sensor consists of
a dye-based photoluminescent O2 -sensing film, a PVDC encapsula-
tion layer, an ITO thin-film heater, a 2 × 2 array of ␮-LEDs embedded
in a PDMS film as a PL excitation light source, red cellophane paper
as an optical filter, an OPD as a PL detector, and an optical isolation
layer for blocking external ambient light. According to our previ-
ous study [44], the sensitivity of the dye-based PL O2 -sensing film
was significantly enhanced by embedding it with TiO2 NPs. O2 can
easily diffuse through the microporous structure of the PS poly-
mer matrix of the O2 -sensing film. The O2 -sensing film was at the
bottom of the wearable bandage-like tcpO2 sensor and directly in
contact with human skin for accurate tcpO2 measurements [46].
The PVDC film above the O2 -sensing film was utilized to mini-
mize the effect of ambient air on tcpO2 measurement from human
skin. The PVDC film had an excellent O2 barrier property as shown
in Fig. S1 to S2 (Supporting Information) [47]. As an additional and
essential component of the O2 sensor we developed previously
[26], the PVDC film significantly enhanced the sensitivity of the
O2 -sensing film (as shown in Fig. S3 in the Supporting Information)
and thus the sensitivity of the wearable sensor due to its excellent
ability to exclude the PL quenching effect of atmospheric O2 on the
inner O2 -sensing film.
The ITO thin-film heater integrated into the bandage-like tcpO2
sensor (Fig. 1a) also played an important role in increasing the
temperature of the skin area in contact with the O2 -sensing film.
Furthermore, instead of the f-OLEDs that degrade with time under
ambient air conditions, a 2 × 2 array of ␮-LEDs connected to a small
and portable external 9 V battery was used as the PL light source of
the O2 -sensing film. The ␮-LED array was arranged such that the
tcpO2 -dependent PL emission of the O2 -sensing film goes through
the center of the ␮-LED array without hindrance and is absorbed
by the active layer of the OPD. The ␮-LED array was embedded into
a thin film of an elastomeric PDMS substrate to make the ␮-LED
array flexible and conformally contact the curves and contours of
human skin without any variation in its light output performance.
As shown in Fig. 1a, the OPD on 50 ␮m-thick PI and the red
cellophane optical filter was easily attached to the surface of the
thin PDMS film hosting the embedded ␮-LED array through van
der Waals force interactions [48]. The OPD was made of organic
semiconductors with inherent mechanical flexibility suitable for
application in a wearable tcpO2 sensor [22]. Therefore, the OPD can
easily be attached to the curved surface of human skin. Further-
more, in comparison to their rigid inorganic counterparts, which
use expensive vacuum fabrication techniques, OPDs have cheap
solution-based fabrication requirements [49]. Black tape serving
as an optical isolation layer covered all other components of the
wearable tcpO2 sensor (Fig. 1a) to eliminate the effect of ambient
light, as shown in Fig. S4 (Supporting Information). All the compo-
nent devices of the wearable tcpO2 sensor were designed to be fully
flexible, allowing them to bend easily with the contours of human
skin, as shown in Fig. 1b.
As shown in the schematic illustration of human skin in Fig. 1b,
tcpO2 is generated from the skin surface due to dissolved O2 in the
tissue and arteriolar O2 partial pressure. O2 generated from the sur-
face of the skin diffuses into the sensing film and is then exposed to
the PtOEP dye molecules. When the photoluminescent dye and O2
molecules collide, photoexcitation, in which metal-ligand charge
transfer (MLCT) that generates an excited triplet state of the dye
4 C.-J. Lim and J.-W. Park / Sensors and Actuators A 298 (2019) 111607

Fig. 1. (a) A schematic diagram of the wearable bandage-like tcpO2 sensor consisting of an ITO thin-film heater (bottom left image), an O2 -sensing film, an encapsulation
layer of PVDC film, a ␮-LED array embedded in PDMS film (upper left image), a red cellophane filter, an OPD, and an optical isolation layer. (b) Digital photograph of the
wearable bandage-like tcpO2 sensor attached to the skin of the foot in which the wires connecting the portable 9 V battery and ␮-LEDs were labeled with the number 1 and
the wires connecting the external power supply and the ITO thin-film heater were labeled with the number 2. The wires connecting the OPD and DAQ module were identified
by the number 3. The bottom illustration in (b) shows how the wearable tcpO2 sensor interacted with the human skin surface. (For interpretation of the references to colour
in this figure legend, the reader is referred to the web version of this article).

molecules takes place, occurs [50]. The lifetime of the excited triplet
state of the PL dye is long enough that as the likelihood of the
dye colliding with an O2 molecule increases, there is a probability
of dynamic quenching occurring; thus, PL-based O2 -sensing films
have significantly higher sensitivity than fluorescence-based sens-
ing films [51].
In the luminescence-based O2 sensor, the optical proper-
ties of the O2 -sensing film, light source, and detector have a
significant influence on the overall performance of the sensor.
The optical properties of all component layers of the wearable
bandage-like tcpO2 sensor are presented in Fig. 2a. As shown
in Fig. 2a, the O2 -sensitive dye absorbed green light from the
␮-LED array, the peak emission wavelength of which is approx-
imately 519 nm, and emitted red PL light with a peak emission
wavelength of approximately 643 nm in relation to the [O2 ]
according to Eq. (1). The poly(3-hexylthiophene-2,5-diyl) and 1-(3-
methoxycarbonyl)propyl-1-phenyl [6,6]C61 (P3HT:PCBM)-based
OPD absorbs the PL emission of the O2 -sensing film after it passes
through the red cellophane filter and then sends photocurrent sig-
nals to the DAQ module.
As shown in Fig. 2a, the FWHM of the ␮-LED emission spectrum
was very narrow, and the signal crosstalk that can be generated due
to the overlapping between the light emission of ␮-the LEDs and
the PL absorption of the OPD was minimized through the use of
the red cellophane optical filter. In other words, the red cellophane
optical filter allowed only the PL emission of the O2 -sensing film to
reach the OPD but excluded the noise coming from the green emit-
ted light of the ␮-LEDs. Fig. 2b shows the J-V characteristics of the
OPD under dark and illumination conditions, indicating that it has
sufficient photovoltaic properties to detect photocurrent changes
induced by the tcpO2 variation. The figure of merit of an optical
luminescence sensor such as our bandage-like wearable tcpO2 sen-
sor is proportional to the performance of the OPD, the responsivity
(R, which is an index of how much current change is induced by a
certain amount of light), and the photocurrent ratio (IL /ID , where
the indices L and D stand for the illuminated and dark current of
the OPD, respectively) [52].
As shown in Fig. 2b, the R of the OPD at 0 V was approxi-
mately 0.053, and the IL /ID in the upper left inset was approximately
591,468, both of which were sufficient for measuring the PL inten-
sities passing through the red cellophane optical filter [45]. The
important experimental parameters for the ␮-LED array and OPD
in the wearable tcpO2 sensor are described in Table I. In addition,
the limit of detection ([O2 ] and tcpO2 of about 1.7% and less than
23 mmHg, respectively) and analyte selectivity of only to O2 of the
tcpO2 sensor were also evaluated and described in Fig. S5 and S6,
respectively (Supporting Information).
As mentioned previously in the Introduction section, one of the
most important factors affecting the sensitivity to tcpO2 is the tem-
perature of the skin surface [53]. Among the components of our
wearable tcpO2 sensor, the ITO thin-film heater increases the sur-
face temperature of the skin. At the normal body temperature of
approximately 37 ◦ , the stratum corneum of the skin acts as a bar-
rier, decreasing the tcpO2 measured from the skin [54]. The elevated
skin temperature changes the structure of the lipid component
of the stratum corneum, which promotes the diffusion of O2 gas
through the skin surface [39]. In addition, the capillary blood vessels
are expanded by the increase in temperature, resulting in increases
in the blood flow velocity on the skin surface and the diffusion rate
of the dissolved gases. In a recent study, relatively low tcpO2 data
were measured using O2 sensors on the skin surface in the absence
of any heating component [26].
As previously shown by others, we also demonstrated in Fig. 3a
and b that the tcpO2 measurements from the skin surface showed
a tendency to increase almost linearly with increasing electrode
and skin temperature [26]. Fig. 3a shows the effect of electrode
and skin temperature variations on the tcpO2 measured using the
commercially available PeriFlux 5000 as the reference sensor. Very
low tcpO2 values of approximately 12 to 18 mmHg were measured
at 37 ◦ , which is the same as the normal human body tempera-
ture. As the temperature of the sensing electrode of the PeriFlux
5000 increased, the measured tcpO2 also increased proportionally,
and a higher tcpO2 of approximately 70 mmHg was measured at a
sensing electrode temperature of approximately 45 ◦ , as shown in
Fig. 3b. In addition, the saturation time of the measured tcpO2 was
approximately 10 min using the PeriFlux 5000, as shown in Fig. 3a,
which was very similar to that obtained by other research groups
[35,36,55,56].
To apply a constant heat to the skin without affecting the optics-
based sensing mechanism of the wearable bandage-like tcpO2
sensor, an ITO thin-film heater was selected as the flexible trans-
parent heater component of the wearable sensor, as depicted in
Fig. 1a. The use of the ITO thin-film heater reduces the risk of acci-
dental electrical shocks to the user of the wearable bandage-like
tcpO2 sensor due to its relatively high electrical sheet resistance
(Rs ) of approximately 82 /sq. compared to that of other flex-
 C.-J. Lim and J.-W. Park / Sensors and Actuators A 298 (2019) 111607 5

Fig. 2. (a) Absorption and emission spectra of the O2 -sensing film, electroluminescence spectrum of the green ␮-LEDs, absorption spectrum of the OPD, and transmission
spectrum of the red cellophane filter. (b) J-V characteristics of the OPD under dark and illumination conditions (inset: logarithmic plot of the corresponding OPD J-V
characteristics). (For interpretation of the references to colour in this figure legend, the reader is referred to the web version of this article).

Fig. 3. (a) The effect of the electrode and skin temperature on the skin tcpO2 measured using the commercially available PeriFlux 5000. (b) Linear relationship between the
measured tcpO2 and the temperature of the PeriFlux 5000 electrode.

ible transparent heaters, such as silver nanowire network-based
heaters. Fig. 4a shows the visible light optical transmittance spec-
tra of the various encapsulation materials and the ITO heater. In the
wearable tcpO2 sensor platform, the encapsulation layer is located
directly above the O2 sensing film (Fig. 1). The PL generated from
the sensing film must reach the organic photodiode (OPD) through
the encapsulation layer such that excellent light transmittance is
required for the encapsulation layer. The optical transmittance of
the PDMS, glass, PI, and PVDC at 650 nm were around 86.2, 90.9,
84.7 and 88.9%, respectively. On the other hand, the ITO thin-film
heater on 50 ␮m-thick colorless PI showed an optical transmittance
of approximately 75.5% in the visible range of light. The inset figure
in Fig. 4a shows the digital photographs of PVDC film and the ITO
heater. As shown in Fig. 4b, the wearable tcpO2 sensor is shown
to operate properly during bending. In the mechanical flexibility
tests to evaluate bending characteristics (Fig. 4c), the Rs of the ITO
thin-film heater started to increase at a bending radius of 9 mm. At
bending radii larger than 9 mm, there was a negligible change in Rs .
Furthermore, the ITO transparent thin-film heater on 50 ␮m-thick
colorless PI showed excellent cyclic bending stability at a bending
radius of 9 mm. As shown in Fig. 4d, the Rs of the heater did not
significantly vary after it was bent for 15,000 bending cycles.
Fig. 5a shows the average temperature variation with time of
the ITO thin-film heater with an applied voltage of 6.2 V and a
corresponding electrical current of 0.03 A. The graph shows that
the ITO thin-film heater had very stable heating properties over a
long period of time. According to Fig. 5b–d, the ITO thin-film heater
showed uniform and constant Joule heating over its entire surface
area of 17 × 17 mm2 during the continuous application of 6.2 V for
60 min [57,58]. Fig. S7 in the Supporting Information presents addi-
tional surface IR images of the ITO thin-film heater during 60 min of
operation. The ITO thin-film heater achieved uniform surface heat-
ing just after 30 s from when the voltage was initially applied. The
ITO thin-film heater helped in the diffusion of tcpO2 through the
skin by uniformly heating the skin area directly under the wearable
tcpO2 sensor, as illustrated in Fig. 1b. A summary of the experi-
mental parameters when the ITO thin-film heater was used as a
component of the wearable tcpO2 sensor is included in Table 1.
Before attaching the sensor to human skin, its O2 -sensing prop-
erties o were optimized and calibrated using a customized gas flow
cell, as shown in Fig. 6a. The O2 content (measured in vol%) in the
gas flow cell was controlled with a mass flow controller directing
the flow of an O2 and nitrogen (N2 ) gas mixture injected into the
gas flow cell. Through the tiny holes on the upper surface of the gas
flow cell chamber, the mixed gas containing O2 was diffused into
the sensing film. The photocurrent from the OPD of the sensor was
transmitted to the LabVIEW software via the photodiode amplifier
and DAQ module. Fig. 6b shows the photocurrent data of the wear-
able tcpO2 sensor in relation to the varying [O2 ]. The photocurrent
value in the absence of O2 means that there was no PL quenching
phenomenon of the dye molecules due to O2 molecules and that
the sensor shows the maximum value.
As the [O2 ] increases, the O2 molecules diffuse into the sensing
film, and the PL intensity of the sensing film decreases in proportion
6 C.-J. Lim and J.-W. Park / Sensors and Actuators A 298 (2019) 111607

Fig. 4. (a) Comparison of the transmittance of the encapsulation layers used in the tcpO2 sensor (glass, PDMS, PI, and PVDC) together with that of the ITO heater. (b) Digital
photograph of the wearable tcpO2 sensor during bending (left) and under illumination from the light source (right). (a) Static bending at various bending radii and (d) cyclic
bending at 9 mm bending radius. The inset in (d) shows a digital image of the ITO thin-film heater during the bending test.

Fig. 5. (a) Long-term heating stability of the ITO thin-film heater during its operation at a 6.2 V applied voltage. (b) IR images of the temperature distribution on the ITO
thin-film heater after (b) 1, (b) 30, and (c) 60 min of operation with the dashed line squares in the images indicating the 17 × 17 mm2 dimensions of the heater.
 C.-J. Lim and J.-W. Park / Sensors and Actuators A 298 (2019) 111607 7

Fig. 6. (a) Schematic diagram of the measurement setup for the performance evaluation of the wearable bandage-like tcpO2 sensor along with the (b) OPD photocurrent
variation over time and (c) Stern-Volmer plot of the wearable bandage-like tcpO2 sensor.

Table 1 molecules inside the sensing film, respectively. f1 and f2 are the
Experimental parameters of each component device composing the wearable
fractions of the O2 molecules uniformly and nonuniformly in con-
bandage-like tcpO2 sensor.
tact with the PtOEP dye molecules, respectively, and f1 +f2 = 1. The
Sensor component Parameters Value numerical parameters of the modified Stern-Volmer Eq. (2) are
devices
described in Table 1. The sensitivity of the O2 -sensing film was
K sv 1 0.0147 measured to be 1.6 at 30% [O2 ] by fitting the relation between
K sv 2 0.3861 the empirical sensitivity variation and [O2 ] presented in Fig. 6c
O2 -sensing film with f1 0.9
with Eq. (2) (data fitting correlation coefficient, R2 , of 0.9951).
embedded TiO2 NPs f2 0.1
Data fitting correlationcoefficient (R2 ) 0.9951 The sensitivity of the sensing film in the [O2 ] range from 0 to
Sensitivity (I0 /I30 ) 1.61 30% was sufficient for the measurement of tcpO2 from human
Operating voltage (V) 9 skin.
2 × 2 ␮-LED array
Average luminescence (cd/m2 ) 147,800
There are various advantages of the intensity-based PL mea-
Dark current (nA/cm2 ) at 0 V 9.08
Flexible OPD IL /ID current ratio at 0 V 591,468 surement approach for the sensing of O2 gas, such as simple data
Responsivity (A/W) 0.053 interpretation, device miniaturization, and low device cost; how-
Operating voltage (V) 6.2 ever, compared to PL lifetime-based methods for sensing O2 gas,
ITO thin-film heater Avg. temperature (◦ ) 44.5 ± 0.15 this approach also has disadvantages. Aside from the PL emitted
Temperature saturation time (s) 30
from the sensing film, intensity-based photoluminescent O2 sen-
sors such as our wearable tcpO2 sensor are also sensitive to the PL
to the contact between the dye and O2 molecules. The relationship activation light source, ambient light and the color of the skin to
of I0 /I with [O2 ] can deviate from the linear function expressed by which they are attached [60]. Consequently, the signal crosstalk in
the Stern-Volmer Eq. (1) due to the uniformity of the dye distri- intensity-based PL O2 sensors due to the effects of the PL activa-
bution inside the sensing film and the nonuniform diffusion of the tion light source and ambient light can be structurally blocked by
O2 gas through the microstructure of the polymer matrix of the optical filters and optical isolation layers, respectively, which we
sensing film. Hence, a two-site model should be used to modify the incorporated into our wearable tcpO2 sensor, as shown in Fig. 1a.
Stern-Volmer Eq. (1) and more accurately express the relationship However, since the varying skin color of wearable tcpO2 sensor
of I0 /I with [O2 ] as: [59] users may also influence the tcpO2 measurements, we defined a
correction coefficient Ksc for the photocurrent measurements as
 −1
I0 f1 f2 described in Table 2 to compensate for the effects of skin color on
= + , (2) our wearable tcpO2 sensor [61].
I 1
1 + KSV [O2 ] 2
1 + KSV [O2 ]
As shown in Fig. 7a, the skin color correction coefficient (Ksc )
where K1 sv and K2 sv are the Stern-Volmer constants when O2 was determined for each user of the wearable tcpO2 sensor by
molecules uniformly and nonuniformly encounter the PtOEP dye photocopying a picture of their skin and calculating the ratio of
8 C.-J. Lim and J.-W. Park / Sensors and Actuators A 298 (2019) 111607

Table 2
Photocurrent correction coefficients for the effects of skin color and temperature.

Experimental parameters Correction coefficient symbol Corrected photocurrent equationa Correction coefficient value

Skin color Ksc I = Ksc x Iraw 0.92 ± 0.007

Temperature Ktemp I = Ktemp x Iraw 1.01 ± 0.001
a
I is the calibrated photocurrent, while Iraw is the raw or as-measured photocurrent.

Fig. 7. Experimental derivation of the correction coefficients for the effects of (a) skin color and (b) temperature on the photocurrent measurements.

Fig. 8. Illustration of the tcpO2 measurement process of a participant with a sensor attached to the skin of a foot during the leg elevation test.

the photocurrent measured from the photocopied skin images to
that of clean white paper, which was the same type of paper as
the paper on which the skin colors were printed. In addition, the
heat emitted by the ITO thin-film heater was expected to affect the
PL emitted by the O2 -sensing film and the photocurrent detected
by the OPD. In addition to their effect on the photocurrent of the
OPD, elevated temperatures have varying effects on the PL quantum
yield, PL quenching, O2 solubility and O2 diffusion in the O2 -sensing
film [62,63]. Interestingly, according to Fig. 7b, the photocurrent of
the wearable tcpO2 sensor in which the O2 -sensing film and OPD
were incorporated showed only linear variation with temperature,
as expressed in Table 2 by the temperature correction factor, Ktemp .
To prove the effectiveness of our sensor in measuring varying
tcpO2 values from human skin, we performed the leg elevation test
as shown in Fig. 8, which is widely used as a diagnostic protocol for
various O2 deficiency-related diseases [64,65]. When the leg is ele-
vated above a certain angle, the tcpO2 at the skin of the leg decreases
because the arterial blood delivery to the limb is delayed [64]. The
leg elevation test was conducted for a total of 60 min in which the
first 11 min were used to stabilize the measurements of the wear-
 C.-J. Lim and J.-W. Park / Sensors and Actuators A 298 (2019) 111607 9

Fig. 9. (a) Photocurrent and corresponding tcpO2 variation over time measured using the bandage-like wearable sensor during the leg elevation test. (b) tcpO2 measurements
from four volunteers participating in the leg elevation test. (c) Comparison of the tcpO2 values measured using the bandage-like wearable tcpO2 sensor and PeriFlux 5000
during the leg elevation test. (d) tcpO2 data with the baseline correction fitting function included in the OriginLab Corp. data analysis software. (e) Comparison of the
baseline-corrected tcpO2 variations with respect to time and multiple leg elevation tests measured using the bandage-like wearable tcpO2 sensor and PeriFlux 5000.
10 C.-J. Lim and J.-W. Park / Sensors and Actuators A 298 (2019) 111607

able tcpO2 sensor according to the results presented in Fig. 3a. The less, while the O2 molecules need comparatively more time to reach
leg was raised at an angle of 60 degrees for 8 min and then lowered and react with the electrochemical electrodes of the PeriFlux 5000
to the level of the test subject’s body for another 8 min, as illustrated [66]. According to the PeriFlux 5000 and wearable tcpO2 sensor,
in Fig. 8. Multiple leg raising and relaxing actions were conducted the extent of tcpO2 reduction from the leg during its elevation was
during the 60 min leg elevation test. 6.18 ± 1.59 and 4.66 mmHg ± 0.17, respectively. Therefore, in addi-
With the sensors attached near the ankle of the test subject, tion to its excellent sensing stability and reversibility over a long
we compared the performance of the wearable tcpO2 sensor to period of time, the wearable tcpO2 sensor was also proven to have
that of the PeriFlux 5000 (a commercially available tcpO2 sensor) better accuracy and a faster reaction rate than the commercially
in measuring the varying tcpO2 during the leg elevation process. available PeriFlux 5000 O2 sensor.
The variation in the photocurrent measured by the wearable tcpO2
sensor during the leg elevation test was corrected using the correc-
4. Conclusion
tion coefficients Ksc and Ktemp (described in Fig. 7 and Table 2), and
the corresponding tcpO2 variation was then determined using the
In this study, we developed a wearable bandage-like tcpO2 sen-
Stern-Volmer plot according to Eq. (2) and Fig. 6. Before convert-
sor consisting of an O2 -sensing film, an encapsulation layer, an
ing the measured photocurrent variation to the correct equivalent
array of ␮-LEDs, an optical filter, an OPD, and an optical isolation
tcpO2 , we placed glass between the skin and the wearable tcpO2
layer. All the components of the sensor were sufficiently flexible
sensor and measured the I0 , which was the baseline of the PL emis-
and can be attached onto the curved skin on any part of the human
sion of the O2 -sensing film at a [O2 ] of 0%. Using the modified
body. The visible light-transparent ITO thin-film heater, showing
Stern-Volmer Eq. (2) with the corresponding constants described
uniform heating at approximately 44.4 ◦ C for 1 h over an area of
in Table 1, the tcpO2 from the skin was determined from the vari-
17 × 17 mm2 , increased the tcpO2 diffusion through the skin with-
ation in I with [O2 ], which includes the skin color and temperature
out affecting the optical signals emitted by the photoluminescent
correction coefficients, Ksc and Ktemp , respectively, as described in
O2 -sensing film and then detected by the OPD inside the wearable
Table 2.
PL-based tcpO2 sensor. Furthermore, an I0 /I30 of approximately 1.6
Fig. 9a shows the I and equivalent tcpO2 values in relation to
was shown to be enough to measure the tcpO2 from the human
the leg elevation test described in Fig. 8. The data presented in
skin surface with the introduction of two correction coefficients
Fig. 9a were taken from the average of three measurements. As
for the user skin color and sensor temperature effects on the PL
seen in the graph, I increased during the lifting of the leg and
emission and detection inside the wearable bandage-like tcpO2
decreased when the leg was dropped from elevation. This result
sensor. Hence, we showed that the wearable bandage-like tcpO2
proved that the tcpO2 measured from the foot decreased when
sensor has a faster response rate and better accuracy than the com-
the leg was raised and was restored to its normal values when
mercially available PeriFlux 5000 tcpO2 sensor in detecting the
the leg was relaxed from elevation. Fig. 9b shows the tendency of
tcpO2 variation from human skin during the leg elevation test. Fur-
the tcpO2 measured using the PeriFlux 5000 to change with leg
thermore, in our future work, we are aiming to minimize if not
elevation and relaxation (the leg dropping to its initial level rel-
eradicate the ambient air-induced degradation of the OPD through
ative to the body) of four different participants. The initial tcpO2
the development of transparent flexible encapsulation films in
values from the four participants were in the range from 50 to
order for our bandage-like tcpO2 sensor to be able operate beyond
90 mmHg. The tcpO2 decreased when the legs of the participants
the current 60 min test and be truly wearable over a long period of
were elevated at an angle of 60 degrees and increased back to
time.
its initial values when the participants lowered or relaxed their
legs.
As shown in Fig. 9c, the relaxed leg had a tcpO2 of approximately Declaration of Competing Interest
74.7 mmHg, which was measured after the sensor was attached
near the ankle of the test participant and stabilized for 10 min. The authors declare that they have no conflict of interest.
However, the I was observed to decrease over time, and accord-
ingly, the tcpO2 increased with it, contrary to the stable constant Acknowledgements
values expected under either elevated or relaxed leg conditions. The
gradual decrease in I with time was due to the gradual degradation This research was supported by the Basic Science Research Pro-
of the OPD and the wearable tcpO2 sensor operated under ambi- gram through the National Research Foundation of Korea (NRF)
ent air conditions and without any encapsulation, as presented in funded by the Ministry of Science, ICT & Future Planning (grant
Fig. S8 and S9, respectively. (Supporting Information). Neverthe- number: 2018R1A2B6001390).
less, both the wearable tcpO2 sensor and PeriFlux 5000 detected
the same trend in the variation of tcpO2 during the leg elevation
Appendix A. Supplementary data
test.
To correct the effects of the small and gradual OPD degradation
Supplementary material related to this article can be found,
with time on the calculated tcpO2 , a baseline correction function
in the online version, at doi:https://doi.org/10.1016/j.sna.2019.
was applied to the tcpO2 variation using OriginLab Corp. data anal-
111607.
ysis software, as presented in Fig. 9d. According to Fig. 9e, the
wearable tcpO2 sensor showed very similar measurements to those
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Biographies
Mr. Chang-Jin Lim is a currently Ph.D candidate in the department of Materials Sci-
ence and Engineering at Yonsei University, Seoul, Korea. He received his B.S and M.S
degrees in Sejong University, Seoul, Korea. His current research interest is wearable
bio-sensors for health monitoring and disease diagnosis.
Professor Jin-Woo Park is a currently professor in the department of Materials
Science and Engineering at Yonsei University, Seoul, Korea. She received her Ph.D
degree in Massachusetts Institute of Technology (MIT) in Cambridge, MA, USA. She
also received her B.S degree in Yonsei University, Seoul, Korea. Her current research
interest is wearable and implantable sensors and power sources.