applied

sciences
Article
Detection of Polystyrene Microplastic Particles in Water Using
Surface-Functionalized Terahertz Microfluidic Metamaterials
Sae June Park 1 and Yeong Hwan Ahn 2, *

1 School of Electronic Engineering and Computer Science, Queen Mary University of London,
London E1 4NS, UK; s.j.park@qmul.ac.uk
2 Department of Physics and Department of Energy Systems Research, Ajou University, Suwon 16499, Korea
* Correspondence: ahny@ajou.ac.kr

Abstract: We propose a novel method for detecting microplastic particles in water using terahertz
metamaterials. Fluidic channels are employed to flow the water, containing polystyrene spheres, on
the surface of the metamaterials. Polystyrene spheres are captured only near the gap structure of the
metamaterials as the gap areas are functionalized. The resonant frequency of terahertz metamaterials
increased while we circulated the microplastic solution, as polystyrene spheres in the solution are
attached to the metamaterial gap areas, which saturates at a specific frequency as the gap areas
are filled by the polystyrene spheres. Experimental results were revisited and supported by finite-
difference time-domain simulations. We investigated how this method can be used for the detection
of microplastics with various solution densities. The saturation time of the resonant frequency
shift was found to decrease, while the saturated resonant frequency shift increased as the solution
density increased.

Keywords: terahertz spectroscopy; metamaterials; sensors; microplastics; lab-on-a-chip

Citation: Park, S.J.; Ahn, Y.H.

Detection of Polystyrene Microplastic
Particles in Water Using 1. Introduction
Surface-Functionalized Terahertz
Microplastics are defined as plastic particles with a size between 1 µm and 5 mm,
Microfluidic Metamaterials. Appl. Sci.
2022, 12, 7102. https://doi.org/
which have become a tremendous issue for the aquatic environment [1,2], and subsequently
10.3390/app12147102
may affect human health through the food chain [2]. For example, microbeads composed of
either polyethylene, polypropylene, or polystyrene have been used in various hygiene prod-
Academic Editors: Matt ucts such as toothpaste, shampoo, conditioner, and body wash and have been found to be
Oehlschlaeger and Mona M. Hella
accumulated in seafood, oceans, freshwater lakes, and rivers [3–6]. It was reported that the
Received: 11 June 2022 typical size of microbeads detected in bottled water is between 1 and 5 µm [7]. Various meth-
Accepted: 12 July 2022 ods including Fourier transform infrared spectroscopy (FTIR), and Raman spectroscopy
Published: 14 July 2022 have been employed to both qualitatively and quantitatively monitor microplastics in
aquatic environments [8–10]. However, their limitations in measurement time, target parti-
Publisher’s Note: MDPI stays neutral
cle size, and complex pre-treatment steps (e.g., density separation) make developing novel
with regard to jurisdictional claims in
in-situ detection methods for microplastics in water environments imperative [2].
published maps and institutional affil-
iations.
Metamaterials are artificially designed structures that interact with electromagnetic
waves at a specific frequency, determined by their geometrical parameters and surrounding
dielectric environment [11–13].√ The inductive–capacitive (LC) resonance mode in metama-
terials, described by f 0 = 1/2π LC, where L is the inductance and C is the capacitance of
Copyright: © 2022 by the authors. the gap area, has been extensively investigated in biosensing research owing to its control-
Licensee MDPI, Basel, Switzerland. lability and high sensitivity [14–22]. It is noteworthy that it has been demonstrated that
This article is an open access article metamaterials operating in the terahertz (THz) frequency range offer ideal platforms for
distributed under the terms and dielectric sensing, more specifically for sensing a few micron-sized target materials such
conditions of the Creative Commons as fungi, and bacteria in ambient and aqueous environments [23–26]. Additionally, the
Attribution (CC BY) license (https:// sensitivity of THz metamaterials as a function of the relative position of the polystyrene
creativecommons.org/licenses/by/ microbead has been recently studied explicitly [27].
4.0/).

Appl. Sci. 2022, 12, 7102. https://doi.org/10.3390/app12147102 https://www.mdpi.com/journal/applsci

Appl. Sci. 2022, 12, 7102 2 of 8

Therefore, it is pertinent to exploit THz metamaterials to develop novel microplastic

sensors working in water environments. As the detection volume of THz metamaterials
is strongly confined to the region near the surface of the metamaterials [15,28], a fluidic
channel with a thin water layer can be integrated into the metamaterials to minimize the
THz absorption from water and flow the microplastic solution on the surface of the metama-
terials [29–36]. Further to this, the gap area of the metamaterials could be functionalized to
capture the microplastics only near the gap structure of the metamaterials where the actual
detection occurs [27]. However, the in situ detection of microplastics using functionalized
THz metamaterials devices in water environments has not been demonstrated yet.
Here, we investigated a new approach to detecting microplastics in aqueous environ-
ments using surface-functionalized THz microfluidic metamaterials that can overcome
the limitation of existing methods based on FTIR and Raman spectroscopy. The fast cir-
culation technique has been employed to enhance the detection speed and sensitivity for
sensing microplastics in aqueous environments. We monitored the change in the reso-
nant frequency of the metamaterials with in situ THz spectroscopy while circulating the
microplastic solution on the surface-functionalized metamaterials using fluidic channel
devices. Finite-difference time-domain (FDTD) simulations were performed to understand
the experimental results. Additionally, we studied the saturation behavior in the resonant
frequency shift as polystyrene-microplastic spheres (PS) were attached to the gap area of
the metamaterials for various PS solution densities.

2. Results and Discussions

Fluidic channel devices that incorporate the functionalized metamaterials were fab-
ricated as shown schematically in Figure 1a,b. The key idea is that the gap areas of
metamaterials are filled by the target materials while the PS solution is continuously circu-
lated as the gap area are functionalized. We note that plasmonic and metamaterial sensors
generally address the density of target material at the sensor surface [16,23,37], while it is
the volume density that is required for sensing in the aqueous environment. We monitored
the change in the resonant frequency of the metamaterials with in situ THz spectroscopy
while injecting the PS solution into the fluidic device. The transmission amplitudes of
THz metamaterial devices were obtained from a conventional in situ THz time-domain
spectroscopy system with an acquisition time of 4 s as described elsewhere [38,39].
A conventional photolithography method was used to pattern metamaterials on a
high-resistivity Si substrate with a thickness of 550 µm. Cr/Au (2 nm/98 nm) metal layers
were deposited to define the arrays of the split-ring resonator (SRR) with a periodicity of
50 µm. The SRR consists of a rectangle ring with outer dimensions of 36 × 36 µm2 , a gap
width of 3 µm and a gap length of 10 µm. The linewidth and the thickness of the SRR were
chosen to be 4 µm and 100 nm, respectively. The geometrical parameters of the metamaterial
unit cell are shown in Figure 1c. Metamaterials were then functionalized to capture the
PS in the water by partially coating an adhesive poly-L-lysine (PLL) layer only in the gap
area, while the rest of the area was coated with an anti-adhesive hexamethyldisilazane
(HMDS) layer [27]. The full-width at half maximum of the metapattern resonance in water
was 130 GHz and we obtained the resonant peak position by using the Gaussian fitting
with an uncertainty of around 1 GHz. To circulate the PS solution on the metasurface, we
fabricated the polydimethylsiloxane (PDMS) fluidic channel with a height of 20 µm and a
width of 2 mm on the metamaterials. The height of the PDMS channel is determined by the
height of the SU-8 mold which was used to fabricate the PDMS channel. The PDMS fluidic
channel was bonded to the surrounding substrate area of the metasurface using the plasma
surface treatment method [31]. We note that the PS solution was circulated through the
fluidic channel using a peristaltic pump with an 80 µL/min rate.
Appl. Sci. 2022, 12, x FOR PEER REVIEW 
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Figure 1. (a) Schematic of surface‐functionalized fluidic THz metamaterials for microplastic detec‐
Figure 1. (a) Schematic of surface-functionalized fluidic THz metamaterials for microplastic detection
tion in the aqueous environment. The gap area is coated by adhesive polymer (pink area), whereas 
in the aqueous environment. The gap area is coated by adhesive polymer (pink area), whereas it is
it is coated by HMDS (blue area), which repels the microplastics. (b) Schematic for the experiments 
coated by HMDS (blue area), which repels the microplastics. (b) Schematic for the experiments in
in which the fluidic metamaterials device is connected to a peristaltic pump for the fast circulation 
which the fluidic metamaterials device is connected to a peristaltic pump for the fast circulation of
of the analyte solution. (c) SRR pattern design used in this work. 
the analyte solution. (c) SRR pattern design used in this work.

Figure 2a shows the separated THz transmission amplitudes of the surface‐function‐
Figure 2a shows the separated THz transmission amplitudes of the surface-functionalized
alized microfluidic metamaterials when the water (black solid line) and PS solution (red 
microfluidic metamaterials when the water (black solid line) and PS solution (red solid line)
solid 
was line)  was 
circulated circulated 
through through 
the fluidic the  fluidic 
channel. channel. 
The inset The  inset 
of Figure of  Figure 
2a shows 2a  shows 
an optical image an  of
optical image of fabricated metamaterials after the circulation of PS solution through the 
fabricated metamaterials after the circulation of PS solution through the fluidic channel. The
fluidic channel. The polarization direction of the incident THz waves is indicated with a 
polarization direction of the incident THz waves is indicated with a white arrow. It was clearly
white arrow. It was clearly shown that the PSs were captured only in the functionalized 
shown that the PSs were captured only in the functionalized gap areas where the PLL layer
gap areas where the PLL layer was deposited, while HMDS‐coated area repelled the PS 
was deposited, while HMDS-coated area repelled the PS in the water [27]. We observed a
in the water [27]. We observed a 15.4 GHz blue‐shift in the resonant frequency from 717 
15.4 GHz blue-shift in the resonant frequency from 717 to 732 GHz with the presence of the PS
to 732 GHz with the presence of the PS in the water. We note that the blue‐shift occurred 
in the water. We note that the blue-shift occurred as the PS in the water decreased the effective
as the PS in the water decreased the effective dielectric constant of the target solution due 
dielectric constant of the target solution due to its low dielectric constant (εPS = 2.56) [27]
to its low dielectric constant (ε
when compared to that of waterPS(ε  = 2.56) [27] when compared to that of water (ε
water = 4.8) [31]. At the low density regime, the blue-shiftwater = 4.8) 

[31]. At the low density regime, the blue‐shift induced by the presence of the PS in the 
induced by the presence of the PS in the water can be quantified by the following relationship:
∆
water can be quantified by the following relationship:  ∆ / coefficient, N
f / f0 = −αNPS (ε PS − ε water )/ε e f f , where α is a sensitivity ε PS is the average
/ , 
where α is a sensitivity coefficient, N
number of PS in the gap areas, and εeffPSis is the average number of PS in the gap areas, and 
the effective dielectric constant near the gap area,
εeff is the effective dielectric constant near the gap area, which is determined by the com‐
which is determined by the combined contributions of the dielectric constants of the substrate
1/2
bined contributions of the dielectric constants of the substrate and the water [23]. ε eff can 

and the water [23]. εeff can be obtained from the relation of/ f water = f air / ε e f f , where fwater
be  obtained  from  the  relation  of  / ,  where  fwater  is  the  resonant  fre‐
is the resonant frequency of the metamaterials with an overlaid water layer on the substrate
quency of the metamaterials with an overlaid water layer on the substrate and fair is the 
and fair is the resonant frequency of the metamaterials without the substrate (air embedded).
resonant frequency of the metamaterials without the substrate (air embedded). We also 
We also note that the fluidic channel device without metamaterials pattern was used as a
note that the fluidic channel device without metamaterials pattern was used as a reference 
reference to mitigate the transmission loss from the water layer.
to mitigate the transmission loss from the water layer. 
To verify and understand our experimental findings, we performed FDTD simula‐
tions  using  commercial  software  (CST  Studio  Suite  2022).  The  time‐domain  solver  was 
used to  minimize the effect  of  the internal  reflection  from the  substrate.  The  geometric 
parameters and periodic boundary conditions were adopted from the metamaterials used 
in the experiments. Dielectric constants of 11.8, 4.8, and 2.56, were used for silicon, water, 
and PS structures, respectively. Two‐ports were assigned to the simulation model to gen‐
erate and receive a linearly polarized incident THz plane wave in the time‐domain. We 
then  performed  a  fast‐Fourier  transform  to  obtain  the  frequency‐domain  transmission 
 frequency of the metamaterials as a function of NPS was investigated in Figure 2c to see 
how the presence of the PS in the water layer affects the resonant frequency shift behavior. 
The amount of blue‐shift increased as the number of PS layers increased, but was satu‐
rated at a specific frequency owing to the confined effective sensing volume of the met‐
Appl. Sci. 2022, 12, 7102
amaterials  near  the  gap  area;  this  is  consistent  with  the  saturation  thickness  of  1.5  4μm 
of 8
estimated for the gap‐width of 3 μm [28]. Conversely, in the monolayer case (for NPS < 30), 
the sensitivity coefficient α of 7.1 × 10−4 was obtained, when fair = 1963 GHz and εeff = 8.66. 

 
Figure 2. (a) Experimentally obtained THz transmission amplitude (normalized) of the surface‐func‐
Figure 2. (a) Experimentally obtained THz transmission amplitude (normalized) of the surface-
tionalized fluidic metamaterials after circulation of the specimen with (red solid line) and without 
functionalized fluidic metamaterials after circulation of the specimen with (red solid line) and
(black solid line) the PS in the water. (inset) Dark‐field microscope image of metamaterials with PS 
without (black solid line) the PS in the water. (inset) Dark-field microscope image of metamaterials
captured in the gap area. (b) Simulated THz transmission amplitude of the metamaterials with a 20 
with PS captured in the gap
μm thick water layer for N area. (b) Simulated THz transmission amplitude of the metamaterials
PS = 0, 30, 90. (c) The resonant frequency of the metamaterials as a function 
with a 20
of NPS.  µm thick water layer for NPS = 0, 30, 90. (c) The resonant frequency of the metamaterials as
a function of NPS .
In order to study the resonant frequency shift behavior of the surface functionalized 
To verify and understand our experimental findings, we performed FDTD simulations
fluidic metamaterials, we performed in situ THz spectroscopy while we were circulating 
using commercial software (CST Studio
the PS solution with a density of 2 × 10 Suite
8 mL 2022). The time-domain solver was used to
−1 through the fluidic channel. Figure 3a shows 

minimize the effect of the internal reflection from the substrate. The geometric parameters
THz transmission amplitude as a function of the circulation time of the PS solution. The 
and periodic boundary conditions were adopted from the metamaterials used in the
blue‐shift behavior was observed as the PLL layer in the gap area attracted the PS in the 
experiments. Dielectric constants of 11.8, 4.8, and 2.56, were used for silicon, water, and
solution. In Figure 3b, we extracted the resonant frequency from Figure 3a as a function 
PS structures, respectively. Two-ports were assigned to the simulation model to generate
of circulation time. We note that a fluctuation was observed in the extracted resonant fre‐
and receive a linearly polarized incident THz plane wave in the time-domain. We then
quency over circulation time that could be attributed to the mechanical motion of the per‐
performed a fast-Fourier transform to obtain the frequency-domain transmission amplitude
istaltic pump [40,41]. Therefore, the fitted curve of the resonant frequency (red line) was 
ofplotted along with the extracted resonant frequency (black square dots). The resonant fre‐
the metamaterials. Figure 2b shows the simulated transmission amplitudes of the
metamaterials with a 20 µm thick water layer for NPS = 0, 30, 90. The resonant frequency of
quency of the metamaterials increased while the PSs in the solution were being attached 
667 GHz was observed for NPS = 0 and the blue-shift of the resonant frequency occurred
to the gap area but was saturated at a specific frequency as there is no change in the effec‐
as NPS increased. A discrepancy between the experimental results and simulations in the
tive dielectric constant of the gap area after a certain level of accumulation of the PS in the 
resonant frequency of the metamaterials was observed, which can be attributed to the
gap area over time, as indicated from our simulation results in Figure 2c. 
fabrication tolerance in the experiments. We note that NPS was first gradually increased
to NPS = 30 with a step of three until there was no space to locate additional PS in the gap
area, then we increased NPS with a step of 30 up to NPS = 120 by adding the additional PS
layer that consists of 30 PS right above the existing PS layer. The resonant frequency of the
metamaterials as a function of NPS was investigated in Figure 2c to see how the presence
of the PS in the water layer affects the resonant frequency shift behavior. The amount of
blue-shift increased as the number of PS layers increased, but was saturated at a specific
frequency owing to the confined effective sensing volume of the metamaterials near the gap
area; this is consistent with the saturation thickness of 1.5 µm estimated for the gap-width
of 3 µm [28]. Conversely, in the monolayer case (for NPS < 30), the sensitivity coefficient α
of 7.1 × 10−4 was obtained, when fair = 1963 GHz and εeff = 8.66.
In order to study the resonant frequency shift behavior of the surface functionalized
fluidic metamaterials, we performed in situ THz spectroscopy while we were circulating
the PS solution with a density of 2 × 108 mL−1 through the fluidic channel. Figure 3a
shows THz transmission amplitude as a function of the circulation time of the PS solution.
The blue-shift behavior was observed as the PLL layer in the gap area attracted the PS
in the solution. In Figure 3b, we extracted the resonant frequency from Figure 3a as a
function of circulation time. We note that a fluctuation was observed in the extracted
resonant frequency over circulation time that could be attributed to the mechanical motion
of the peristaltic pump [40,41]. Therefore, the fitted curve of the resonant frequency (red
line) was plotted along with the extracted resonant frequency (black square dots). The
resonant frequency of the metamaterials increased while the PSs in the solution were being
attached to the gap area but was saturated at a specific frequency as there is no change in
the effective dielectric constant of the gap area after a certain level of accumulation of the
PS in the gap area over time, as indicated from our simulation results in Figure 2c.
Appl. Sci. 2022, 12, 7102
Appl. Sci. 2022, 12, x FOR PEER REVIEW  5 of8 8
5  of 
 

 
Figure 3. (a) A color‐scale plot of the normalized transmission amplitude as a function of circulation 
Figure 3. (a) A color-scale plot of the normalized transmission amplitude as a function of circulation
time of the PS solution. (b) The extracted (black dots) resonant frequency as a function of the circu‐
time of the PS solution. (b) The extracted (black dots) resonant frequency as a function of the
lation time. Red line indicates the fitted curve to the experimental data. 
circulation time. Red line indicates the fitted curve to the experimental data.

To investigate the effect of the PS solution density on the saturation behavior of the 
To investigate the effect of the PS solution density on the saturation behavior of
resonance, we performed the same in situ THz spectroscopy again but for various PS so‐
the resonance, we performed the same in situ THz spectroscopy again but for various
PS solution densities (2, 1 × 10
lution densities (2 × 10 8
× 108, 3 × 10
9
, 1 × 10, 6 × 10
9 9
, 3 ×  mL
9
109 , 6). In Figure 4, the saturation time (T
−1
× 109 mL−1 ). In Figure 4, the satu- sat) 

of the resonant frequency shift and the saturated resonant frequency (f
ration time (Tsat ) of the resonant frequency shift and the saturated resonant frequency max) were plotted 

as a function of the PS solution density. Here, T
(∆f sat corresponds to the time when the reso‐
max ) were plotted as a function of the PS solution density. Here, Tsat corresponds to the
nant frequency shift reaches the half of the maximum frequency shift. f–time curves for 
time when the resonant frequency shift reaches the half of the maximum frequency shift.
different solution densities were best fitted with the sigmodal function of 
∆f –time curves for different solution

densities were best fitted with the sigmodal ∆ 1
∆ function
1/∆1f = ∆/f max 1 −, where p is the exponent. The saturation time of 16.6 min was obtained 
of p
1/ 1 + (t/Tsat ) , where p is the exponent. The saturation time of
with the PS solution density of 2 × 10
16.6 min was obtained with the PS solution
8 mL−1, which decreased to 18.5 s with the PS solution 
density of 2 × 108 mL−1 , which decreased
density of 6 × 10 9  mL −1 . We note that FTIR and Raman spectroscopy have been often em‐
to 18.5 s with the PS solution density of 6 × 109 mL−1 . We note that FTIR and Raman
ployed to detect microplastics in water [8–10]. However, a liquid sample containing mi‐
spectroscopy have been often employed to detect microplastics in water [8–10]. However,
croplastics must go through a pre‐treatment step called density separation. The density 
a liquid sample containing microplastics must go through a pre-treatment step called
separation 
density extracts The
separation. microplastics  from  the extracts
density separation sample microplastics
liquid  by  either 
fromletting  microplastics 
the sample liquid by
float or sink in solutions with higher or lower densities than the microplastics [8–10]. This 
either letting microplastics float or sink in solutions with higher or lower densities than
process makes the detection techniques employing FTIR and Raman spectroscopy a time‐
the microplastics [8–10]. This process makes the detection techniques employing FTIR
consuming job, which often takes 5 h to up to 1 day [8]. On the other hand, we could detect 
and Raman spectroscopy a time-consuming job, which often takes 5 h to up to 1 day [8].
microplastics in water with in situ THz spectroscopy by using surface‐functionalized flu‐
On the other hand, we could detect microplastics in water with in situ THz spectroscopy
idic metamaterials. The saturated resonant frequency shift increased further from 15 to 24 
by using surface-functionalized fluidic metamaterials. The saturated resonant frequency
GHz as we increased the PS solution density from 2 × 10
shift increased further from 15 to 24 GHz as we increased
8 to 6 × 109 mL−1 even though it 
the PS solution density from
2was expected that the number of the accumulated PS in the gap area would be similar for 
× 108 to 6 × 109 mL−1 even though it was expected that the number of the accumulated
different PS solution densities. This could be explained by the fact that the effective die‐
PS in the gap area would be similar for different PS solution densities. This could be
lectric constant of the surrounding PS solution also decreases as the PS solution density 
explained by the fact that the effective dielectric constant of the surrounding PS solution
increases, owing to the low dielectric constant of the PS compared to the water, leading to 
also decreases as the PS solution density increases, owing to the low dielectric constant
a further increase in the saturated resonant frequency shift. It is noteworthy that we re‐
of the PS compared to the water, leading to a further increase in the saturated resonant
ported the relationship between the dielectric constant of overlaid liquid and the resonant 
frequency shift. It is noteworthy that we reported the relationship between the dielectric
frequency shift in our previous study [31]. For instance, we estimated the effective dielec‐
constant of overlaid liquid and the resonant frequency shift in our previous study [31]. For
tric constant for the 6 × 10
instance,
9 mL−1 case from the saturated frequency shift and found that 
we estimated the effective dielectric constant for the 6 × 109 mL−1 case from the
the dielectric constant decreased by −1.0 when compared to the water case. 
saturated frequency shift and found that the dielectric constant decreased by −1.0 when
compared to the water case.
 Appl. Sci. 2022, 12, x FOR PEER REVIEW 
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Figure 4. Saturation time of the resonant frequency shift (black square dots), and saturated resonant 
Figure 4. Saturation time of the resonant frequency shift (black square dots), and saturated resonant
frequency shift (red square dots) as a function of the PS solution density. Error bars indicate the 
frequency shift (red square dots) as a function of the PS solution density. Error bars indicate the
standard deviation extracted from the fitting process. 
standard deviation extracted from the fitting process.

3.3. Conclusions 
Conclusions
We investigated a novel real‐time microplastic sensor in a water environment by per‐
We investigated a novel real-time microplastic sensor in a water environment by
forming  in in
performing situ 
situTHz 
THzspectroscopy 
spectroscopyon 
on surface‐functionalized  fluidic metamaterials.
surface-functionalized fluidic metamaterials. PSs
PSs 
were only captured in the gap structure of the metamaterials as the PLL layer in the gap 
were only captured in the gap structure of the metamaterials as the PLL layer in the gap
attracted the PS in the water, while HMDS coated area repelled the PS. We showed that
attracted the PS in the water, while HMDS coated area repelled the PS. We showed that 
the resonant frequency of metamaterials increased as the PSs were captured in the gap
the resonant frequency of metamaterials increased as the PSs were captured in the gap 
area. Also, we monitored the resonant frequency change while we were circulating the
area. Also, we monitored the resonant frequency change while we were circulating the PS 
PS solution through the fluidic channel and extracted the saturation time of the resonant
solution through the fluidic channel and extracted the saturation time of the resonant fre‐
frequency shift, and the saturated resonant frequency shift for various PS solution densities.
quency shift, and the saturated resonant frequency shift for various PS solution densities. 
Experimental results were confirmed and supported by FDTD simulation results. We
Experimental results were confirmed and supported by FDTD simulation results. We suc‐
successfully demonstrated the detection of the PS in water with in situ THz spectroscopy
cessfully demonstrated the detection of the PS in water with in situ THz spectroscopy by 
by using surface-functionalized fluidic metamaterials. We anticipate that this work will
using surface‐functionalized fluidic metamaterials. We anticipate that this work will con‐
contribute to the development of real-time, on-site, cost-efficient, and highly sensitive
tribute to the development of real‐time, on‐site, cost‐efficient, and highly sensitive micro‐
microplastic sensors to tackle the absence of efficient microplastic sensors working in an
plastic sensors to tackle the absence of efficient microplastic sensors working in an aque‐
aqueous environment.
ous environment. 

Author Contributions: Conceptualization,
Author Contributions: Conceptualization, Y.H.A.;
Y.H.A.; Data
Data curation,
curation, S.J.P.;
S.J.P.; Formal
Formal analysis,
analysis, S.J.P.;
S.J.P.; 
Funding acquisition, Y.H.A.; Investigation, S.J.P. and Y.H.A.; Methodology, Y.H.A.; Writing—original
Funding acquisition, Y.H.A.; Investigation, S.J.P. and Y.H.A.; Methodology, Y.H.A.; Writing—orig‐
draft, S.J.P. and Y.H.A. All authors have read and agreed to the published version of the manuscript.
inal draft, S.J.P. and Y.H.A. All authors have read and agreed to the published version of the man‐
uscript.  This work was supported by the Midcareer Researcher Program (2020R1A2C1005735) and
Funding:
Basic Science Research Program (2021R1A6A1A10044950) through a National Research Foundation
Funding: This work was supported by the Midcareer Researcher Program (2020R1A2C1005735) and 
grant funded by the Korea Government.
Basic Science Research Program (2021R1A6A1A10044950) through a National Research Foundation 
grant funded by the Korea Government. 
Data Availability Statement: Not applicable.
Institutional Review Board Statement: 
Conflicts of Interest: The authors declare  no conflict of interest.
Informed Consent Statement:   
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