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Sensors and Actuators A 331 (2021) 112876

Contents lists available at ScienceDirect

Sensors and Actuators A: Physical


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

Semi-transparent reduced graphene oxide temperature sensor on


organic light-emitting diodes for fingerprint liveness detection of
smartphone authentication
Hanyung Jung a , Hyunkoo Lee b,∗
a
Department of Electrical and Electronics Engineering, Seoyeong University, Gyeonggi-do, Republic of Korea
b
Department of Electronics Engineering, Sookmyung Women’s University, Seoul, 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 report a semi-transparent temperature sensor for fingerprint liveness detection on an organic light-
Received 4 March 2021 emitting diode (OLED). Solution-processable graphene oxide was coated between two indium tin oxide
Received in revised form 19 May 2021 electrodes on a glass substrate, and a semi-transparent reduced graphene oxide (rGO) temperature sen-
Accepted 29 May 2021
sor was successively fabricated through graphene oxide (GO) reduction using a laser source. The rGO
Available online 2 June 2021
temperature sensor showed a resistance variance characteristic of 80 % compared to the initial resis-
tance when heated from 15 ◦ C to 170 ◦ C. When finger was touched on the rGO temperature sensor, the
Keywords:
resistance variation was 0.5 % and 7 % at 35 ◦ C and 50 ◦ C, respectively. In addition, GO was coated on
Graphene oxide
Reduced graphene oxide
the light-emitting side of green phosphorescent OLEDs to investigate the damage caused by photother-
Organic light-emitting diode mal reduction energy. The OLEDs irradiated by the laser source for GO reduction showed nearly the same
Laser irradiation current–voltage characteristics and electroluminescence spectrum as the device without laser irradiation,
Temperature sensor although the luminance of the device decreased due to the absorption of rGO.
Fingerprint sensor © 2021 Elsevier B.V. All rights reserved.

1. Introduction fluoride–trifluoroethylene (P(VDF-TrFE)) copolymer [4]. There-


fore, a transparent temperature sensor that can be applied
Biometric authentication is becoming increasingly popular in to a smartphone was manufactured using transparent and
mobile devices [1]. In recent smartphones, fingerprint recognition temperature-sensitive materials such as graphene [5].
has gradually expanded to mobile display screens with advances Graphene, reduced graphene oxide (rGO), and nanoporous car-
in display technology [2]. The Samsung Galaxy S10 smartphone, bon materials have received a lot of attention owing to their
launched in 2019, uses an ultrasonic method for organic light- transparency and high conductivity [6–21]. In particular, rGO thin
emitting diode (OLED) display, and the Samsung Galaxy A50, films reduced from graphene oxide (GO) are suitable for opti-
launched in 2020, uses an optical method of on-screen fingerprint cal transparency and electrical conductivity [22–32]. In addition,
recognition. The fingerprint recognition method on the smartphone because rGO is sensitive to temperature changes, it can easily
screens has gradually expanded to large screens, and the temper- measure the temperature variance when fingerprints are being
ature measurement of a living body can function as an important authenticated on a mobile display screen.
factor to prevent the spoofing and forgery of fingerprints during Here, we report semi-transparent temperature sensors fab-
biometric authentication. Therefore, a temperature sensor needs to ricated using rGO sheets and patterned indium tin oxide (ITO)
be fabricated on a display screen to check the liveness of fingerprint electrodes on a glass substrate. The temperature sensor was simu-
authentication. lated as a fingerprint sensor on the display screen of a smartphone,
Commercial temperature sensors have a wide operating range and the temperature changes were detected through a finger touch.
and high responsiveness [3]. However, it is difficult to apply During real-time fingerprint sensing, it can simultaneously mea-
them on display screens because they are commonly made of sure finger temperature to check the finger liveness and enhance
opaque materials such as platinum, copper, and poly(vinylidene the level of security for biometric authentication [33]. In addition,
we reduced GO on green phosphorescent OLEDs using a laser light
source. The GO layer was successively reduced to rGO without dam-
∗ Corresponding author.
aging the OLEDs.
E-mail address: lhk108@sookmyung.ac.kr (H. Lee).

https://doi.org/10.1016/j.sna.2021.112876
0924-4247/© 2021 Elsevier B.V. All rights reserved.
H. Jung and H. Lee Sensors and Actuators A 331 (2021) 112876

Fig. 1. Temperature sensor fabrication process flow of laser light irradiation. (a) Glass substrate with ITO pattern with gap of 1 mm, (b) GO droplet via drop casting, (c) laser
light irradiation of GO, (d) the fabricated rGO sheet.

Table 1 hexaazatriphenylene hexacarbonitrile (HAT-CN, 10 nm) as the


Concentration calculation of GO material on glass.
hole-injection layer, 1,1-Bis((di-4-tolylamino)phenyl)cyclohexane
GO material mass Calculation (TAPC, 50 nm) as the hole-transport layer, 4,4 ,4 -tri(N-
GO solution concentration 0.5 mg/mL carbazolyl)triphenylamine (TcTa, 10 nm) as the electron-blocking
GO solution drop on sensor 0.002 mL layer, 2,6-bis(3-(carbazol-9-yl)phenyl)pyridine (26DCzPPy,
Dried GO on sensor 0.001 mg 10 nm) doped with tris(2-phenylpyridine)iridium(III) (Ir(ppy)3 ,
GO droplet radius 0.6 mm 7 %) as the green phosphorescent emitting layer, tris(3-(3-
GO concentration 88.5 ␮g/cm2
pyridyl)mesityl)borane (3TPYMB, 25 nm) as the electron-transport
layer, lithium (Li)-doped 3TPYMB (30 nm) and lithium fluoride
2. Materials and methods (LiF, 1 nm) as the electron-injection layers, and aluminum (Al,
100 nm) as the cathode. Li was purchased from a commercial com-
2.1. rGO temperature sensors pany (SAES Getters S.p.A., Italy) and evaporated at approximately
870 ◦ C. The 3TPYMB and Li were simultaneously co-evaporated,
To fabricate the rGO temperature sensor, a transparent rigid and their deposition rates were approximately 0.6 Å/s and 0.03 Å/s,
glass was prepared to prevent deformation by external forces, as respectively. During the deposition of the doping layers, the
shown in Fig. 1. ITO electrodes were patterned as external terminals deposition rates of both the host and dopant materials were
on a glass substrate, and a gap of 1 mm was formed between the two controlled using a quartz crystal oscillator. The fabricated OLEDs
electrodes. A total of 0.002 mL of GO solution (Graphene Supermar- were transferred to a nitrogen-filled glove box, where they were
ket, 0.5 mg/mL concentration) was drop-cast over the gaps between encapsulated using a UV-curable epoxy and a glass cap with a
the electrodes. A total of 0.001 mg of GO solution droplets were moisture absorbent. The emission area of the fabricated devices
dried at 20 ◦ C for 20 h. The dried GO concentration was 88.5 ␮g/cm2 , was 2 mm × 2 mm.
as shown in Table 1. The GO sheet was reduced by laser irradiation The current density–voltage (J–V) characteristics were mea-
from the top. After GO reduction, the edge of the ITO electrodes was sured using a source-measure unit (Keithley-2450, Tektronics,
coated with silver paste (CANS, ELCOAT; resistivity 10−4 ·cm) to U.S.A.), and the luminance (L) and electroluminescence (EL) spec-
minimize the contact resistance between the electrodes. The exter- tra were examined using a spectroradiometer (CS-2000, Konica
nal circuit was connected to a multimeter (GDM-8351, GWINSTEK, Minolta, Japan). The J–V–L measurements of the OLEDs were con-
Taiwan) for resistance measurement. Both the rGO resistance and ducted at room temperature (∼293 K) in a dark box. The efficiencies
temperature of the device were simultaneously measured using were calculated using luminance, current density, and EL spectra.
a commercial multimeter and a temperature sensor, respectively.
The optical transmittance of the rGO on ITO-patterned glass was 3. Results & discussion
measured using an ultraviolet–visible–near-infrared (UV–vis–NIR)
spectrophotometer (Lambda 750, PerkinElmer, U.S.A.). After applying light source irradiation for GO reduction,
rGO was verified via Raman spectroscopy and X-ray photo-
2.2. Green phosphorescent OLEDs electron spectroscopy (XPS) measurements. The ID /IG (=1.0365)
ratios of GO in the Raman spectrum increased to the ID /IG
ITO-patterned glass substrates were sequentially cleaned with (=1.1240) ratios of rGO, indicating a better graphitization of
sulfuric acid, acetone, and methanol, followed by rinsing with rGO than that of GO, as shown in Fig. 2(a). The oxygen-
deionized water. After drying the substrates, all organic materi- containing functional groups in GO were removed, resulting in
als and top cathode metals were deposited in succession using the re-establishment of sp2 hybridized C C bonds. The XPS mea-
the vacuum thermal evaporation method without breaking the surements showed that both C O (286.5 eV) and C O (287.8 eV)
vacuum. The device consisted of ITO as the anode, 1,4,5,8,9,11- bonding of GO decreased, as shown in Fig. 2(b). Therefore,

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H. Jung and H. Lee Sensors and Actuators A 331 (2021) 112876

Fig. 2. GO and rGO obtained through light irradiation reduction: (a) Raman spectra of D peak (1350 cm−1 ) and G peak (1580 cm−1 ) (b) XPS spectra.

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H. Jung and H. Lee Sensors and Actuators A 331 (2021) 112876

Fig. 4. Resistance and variance percentage of (a) first temperature sweep from 15 ◦ C
to 170 ◦ C and (b) 10th temperature sweep from 15 ◦ C to 170 ◦ C.

Fig. 3. (a) Optical transmittance of rGO/ITO/Glass (Inset: photograph of


rGO/ITO/Glass, red arrow: ITO, black arrow: rGO). (b) Resistance variance of rGO The rGO film was fabricated on ITO (150 nm)/glass (0.7 mm) to
temperature sensor at 40 ◦ C (For interpretation of the references to colour in this measure the optical transmittance, as shown in Fig. 3(a). The optical
figure legend, the reader is referred to the web version of this article). transmittance of rGO/ITO/glass was approximately 54 % at 550 nm,
which is sufficient for display applications. The resistance value
Raman spectroscopy and XPS measurements indicated that the of the manufactured rGO temperature sensor was measured after
oxygen-containing functional groups in GO were significantly stabilization for 1 h at 29 % humidity. Resistance variance, R, was
removed. calculated as R0 – R divided by R0 , where R0 and R are the initial

Fig. 5. Schematic cross-sectional structure of (a) commercial OLED mobile display panel with on-display fingerprint sensor. (b) rGO temperature sensor with buffer layer of
polyimide film.

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H. Jung and H. Lee Sensors and Actuators A 331 (2021) 112876

Fig. 6. Resistance variance of rGO temperature sensor during finger touch at (a) 15 ◦ C, (b) 25 ◦ C, (c) 32 ◦ C, (d) 35 ◦ C, (e) 40 ◦ C, and (f) 50 ◦ C. Touch on (first arrow) and off
(second arrow).

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H. Jung and H. Lee Sensors and Actuators A 331 (2021) 112876

Fig. 7. (a) Device structure of OLEDs with rGO layer, (b) J–V–L characteristics, (c) luminous current efficiency as a function of luminance, (d) EL spectra (inset: photograph of
green-emitting OLEDs) of OLEDs with (w/) and without (w/o) rGO layers.

resistance and resistance at a specific temperature, respectively, as sensor had a large resistance change at a temperature similar to
follows: that of the body temperature in the range of 20 ◦ C–40 ◦ C.
Commercial touch-integrated OLED display panels are covered
R0 − R with glass on the top and are composed of several hundred microm-
R = × 100 (%) (1)
R0 eters, as shown in Fig. 5(a). Even the most recent foldable display
panels are made of ultra-thin glass of tens of micrometers. In the fin-
According to Eq. (1), the change in resistance variance was under
gerprint sensor of photodiode method on the smartphone display
1 % at 40 ◦ C for 3 h 30 min, as shown in Fig. 3(b). Because the
screen, the photo signal of the fingerprint was operated by passing
resistance fluctuation for checking the liveness of the finger touch
through the transparent touch sensor panel and the OLED display
occurred within a second, the fluctuation of less than 1 % for 3 h
panel. Therefore, the rGO temperature sensor can be used for fin-
was sufficient.
gerprint authentication when trying to identify fake fingerprints,
The manufactured rGO temperature sensor was heated from
such as silicon or fingerprint photos.
15 ◦ C to 170 ◦ C using a hot plate. The resistance of the rGO sen-
The rGO sensor measured real-time temperature using a poly-
sor was measured from 200 k to 50 k at 15 ◦ C to 170 ◦ C in
imide film of Kaptone® tape of 100 ␮m instead of a glass as a
the first temperature sweep, just after manufacture, as shown in
protective cover glass for the mobile phone, as shown in Fig. 5(b).
Fig. 4(a). The resistance of the rGO temperature sensor decreased
When the finger was touched on the polyimide film, a tempera-
as the temperature increased. This was due to the improved charge
ture change occurred within a second. This temperature change
transport properties with the increase in temperature in rGO, which
was continuously evaluated when the rGO temperature sensor
was mainly dominated by the hopping transport mechanism [34].
was touched under various temperature conditions, as shown
The change percentage in resistance was obtained using Eq. (1)
in Fig. 6(a)–(f). At 15 ◦ C and 25 ◦ C, when the temperature was
to calculate the resistance variance rate. The resistance of the rGO
lower than that of the finger skin, which was adjusted to approxi-
temperature sensor changed from 600 k to 120 k at the 10th
mately 33 ± 1 ◦ C [35], the resistances of the rGO temperature sensor
temperature sweep when the temperature increased from 15 ◦ C to
increased to 3.4 % and 2.7 % of the initial resistances, respectively,
170 ◦ C, as shown in Fig. 4(b), which was the same as the first tem-
according to Eq. (1), as shown in Fig. 6(a) and (b). The increase in
perature sweep range. In the 10th temperature sweep from 15 ◦ C to
temperature of the rGO temperature sensor showed a decrease in
170 ◦ C, the rate of temperature variance obtained using Eq. (1) was
resistance because a relatively higher finger temperature resulted
the same as that of the first temperature sweep, whereas the resis-
in an increase in rGO temperature. At 32 ◦ C and 35 ◦ C, when the tem-
tance value increased three times. When the temperature changed
perature was close to the finger temperature, the resistances of the
from 20 ◦ C to 40 ◦ C, the resistance variance rate of 21.7 % was
rGO temperature sensor changed by 0.3 % and −0.8 %, respectively.
obtained using Eq. (1). However, when the temperature changed
When the difference between the rGO temperature sensor and the
from 120 ◦ C to 140 ◦ C, which was a relatively high temperature, the
finger temperature was low, the fluctuation in the resistance values
resistance variance rate changed to 4.4 %. This was advantageous
was also low, as shown in Fig. 6(c) and (d). When the sensor tem-
in the detection of body temperature because the rGO temperature

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H. Jung and H. Lee Sensors and Actuators A 331 (2021) 112876

perature was higher than the finger temperature, the resistances Acknowledgements
of the rGO temperature sensor changed in the negative direction
of the initial resistances, as shown in Fig. 6(e) and (f). At relatively This research was partly supported by the Sookmyung Women’s
high temperatures of 40 ◦ C and 50 ◦ C, the resistances changed by University Research Grants (1-2103-2001) and in part by the Elec-
−2.5 % and −7.5 %, respectively. Consequently, the rGO temper- tronics and Telecommunications Research Institute (ETRI) grant
ature sensor showed a reversal of the resistance variance based funded by the Korean government (21ZB1200) and in part by the
on a finger temperature of 33 ◦ C. The resistance variance increased Korea Evaluation Institute of Industrial Technology (KEIT) grant
as the difference between the rGO temperature sensor and finger funded by the Ministry of Trade, Industry & Energy (MOTIE, Korea)
temperature increased. (20015805, Development of material parts and processing tech-
The GO layer was coated and reduced on a glass substrate with nology for post InP fluorescence quantum dot) and in part by the
a green phosphorescent OLED to test the influence of laser irradi- National Research Foundation of Korea (NRF) grant funded by the
ation, as shown in Fig. 7(a). The current density of the device with Korea government (MSIT) (No. 2021R1F1A1045517).
the rGO layer was nearly the same as that of the device without the
rGO layer, as shown in Fig. 7(b). For instance, the current densities
of the device without and with the rGO layers were 1.51 mA/cm2 References
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[24] Y. Zhu, S. Murali, M.D. Stoller, A. Velamakanni, R.D. Piner, R.S. Ruoff, Hanyung Jung received the B.S. and the M.S. degree in
Microwave assisted exfoliation and reduction of graphite oxide for Electronics Engineering from Kyungpook National Uni-
ultracapacitors, Carbon 48 (2010) 2118–2122, http://dx.doi.org/10.1016/j. versity in 2000 and 2005, respectively. He worked as a
carbon.2007.02.034. circuit design engineer in LG Display Company for Mon-
[25] H. Jung, H. Lee, J. Lee, Combinational reduction of graphene oxide via coherent itor development, Korea from 2005 to 2009. He received
and incoherent light irradiation for flexible supercapacitors, Diam. Relat. his Ph.D. degree in 2014 from Seoul National University
Mater. 113 (2021), http://dx.doi.org/10.1016/j.diamond.2020.108237, 03, with supercapacitors and minor in MEMS. He worked as a
108237. staff engineer in SAMSUNG Display Company from 2014
[26] H. Jung, C.V. Cheah, N. Jeong, J. Lee, Direct printing and reduction of graphite for the photoelectric sensors and flexible display. He has
oxide for flexible supercapacitors, Appl. Phys. Lett. 105 (2014), 053902, http:// been with Seoyeong University as an assistant professor
dx.doi.org/10.1016/j.carbon.2007.02.034. since 2019. He is interested in nanotechnology and sensor
[27] B. Saha, S. Baek, J. Lee, Highly sensitive bendable and foldable paper sensors applications.
based on reduced graphene oxide, ACS Appl. Mat. Interfaces. 5 (2017)
4658–4666, http://dx.doi.org/10.1016/j.carbon.2007.02.034. Hyunkoo Lee received his B.S. and M.S. Electrical Engi-
[28] G. Williams, B. Seger, P.V. Kamat, TiO2 graphene nanocomposites UV assisted neering degrees from Seoul National University in 2004
photocatalytic reduction of graphene oxide, ACS Nano 2 (7) (2008) and 2006, respectively. He was a junior researcher in the
1487–1491, http://dx.doi.org/10.1021/nn800251f. Monitor Circuit Design Team of LG Display from 2006 to
[29] R. Mukherjee, A.V. Thomas, A. Krishnamurthy, N. Koratkar, Photothermally 2009. He received his Ph.D. Electrical Engineering degree
reduced graphene as high-power anodes for lithium-ion batteries, ACS Nano in 2013, also from Seoul National University. He was a
6 (2012) 7867–7878, http://dx.doi.org/10.1021/nn800251f. senior researcher from 2013 to 2020 in the Reality Display
[30] M.F. El-Kady, V. Strong, S. Dubin, R.B. Kaner, Laser scribing of Research Section of Electronics and Telecommunications
high-performance and flexible graphene-based electrochemical capacitors, Research Institute (ETRI). He has been with Sookmyung
Science 335 (2012) 1326–1330, http://dx.doi.org/10.1126/science.1216744. Women’s University as an assistant professor since 2020.
[31] Z. Chen, C. Lu, Humidity sensors: a review of materials and mechanisms, Sens. His research interests include optoelectronics devices
Lett. 3 (2005) 274–295, http://dx.doi.org/10.1166/sl.2005.045. such as OLEDs, quantum dot-LEDs, and microdisplays.
[32] D. Zhang, D. Wang, P. Li, X. Zhou, X. Zong, G. Dong, Facile fabrication of
high-performance QCM humidity sensor based on layer-by-layer
self-assembled polyaniline/graphene oxide nanocomposite film, Sens.
Actuators B Chem. 255 (2018) 1869–1877, http://dx.doi.org/10.1016/j.snb.
2017.08.212.

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