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TiO2 Nanodisk Arrays as All-Dielectric Huygens’ Metasurfaces for

Engineering the Wavefront of Near-UV Light
Tse-An Chen, Yu-Cheng Chou, Tsung-Yu Huang, Yu-Jung Lu, Yu-Ping Kuang, and Ta-Jen Yen*
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ABSTRACT: Electromagnetic components are important for

ultraviolet (UV) applications. However, due to the limitation in
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the materials’ intrinsic responses, there are fewer electromagnetic

components in high-frequency regimes than in low-frequency ones.
Conventional UV components manipulate the wavefront via
geometric phase accumulation; thus, they are significantly bulky
and inefficient. In this study, we demonstrate all-dielectric
Huygens’ metasurface (ADHMS) at a near-ultraviolet (NUV)
regime. The NUV-ADHMS is comprised of resonant titanium
dioxide (TiO2) nanodisks, with the ultrathin thickness of the fifth
wavelength. In addition, by modulating the diameter of the
resonant TiO2 nanodisks, we can simultaneously excite and control
both electric and magnetic dipoles, achieving a powerful wavefront
engineering of the near-unity transmittance and a full range of the 2π phase coverage. Finally, we employed the NUV-ADHMS to
bend a normal incident beam, demonstrating a deflection angle of 11° at a wavelength of 405 nm.
KEYWORDS: Huygens’ metasurface, flat optical devices, beam bending, phase manipulation, ultraviolet

■ INTRODUCTION
Recently, ultraviolet (UV) devices have attracted considerable
guiding meta-atoms,18,23,39 geometric phases,18,20,23,28,30,32,40,41
and Huygens’ metasurfaces (HMSs).8,42−48 However, these
attention in various fields, such as deep/extreme UV mechanisms have some drawbacks. For example, resonating
lithography systems in semiconductor fabrication industries, meta-atoms appear useful only for a reflective-type metasur-
sterilization in medical and pharmaceutical industries, and face, waveguiding meta-atoms require thick dimensions for
wireless communication in military usage. For these UV accumulating a sufficient phase (i.e., at least 2 to 3λ),
applications, optical components are certainly important for geometric phases suffer from a limited polarization choice
engineering the wavefront of UV light. Conventional optical (i.e., circular polarization only), and HMS is limited to
materials with lower intrinsic losses/larger refraction indices.
components manipulate the wavefront via geometric phase
Due to the high-frequency nature of UV light, natural materials
accumulation, which causes a series of challenges, such as a
show little response to it or possess larger intrinsic losses/lower
difficult fabrication process,1−4 a spherical aberration for
refraction indices, thus inhibiting its practical application.
lenses,5,6 and bulk but less focusing power at UV.7 To
Moreover, for HMS, the low height (∼1/4λ) of meta-atoms
overcome these challenges, metasurfaces have recently
are appealing for the realization of tunable metasurfaces with
emerged, which seem to be a promising solution. Metasurfaces
incorporated active materials. Thus, in this study, we designed
are artificially constructed structures with subwavelength
a series of titanium dioxide (TiO2) nanodisks to present an all-
feature sizes and thickness, making it possible to harness the
dielectric Huygens’ metasurface (ADHMS) at a near-ultra-
amplitude,8−11 phase,12−19 and polarization of electromagnetic
violet (NUV) regime. By simultaneously exciting and further
waves.20−22 Using the compelling concept of metasurfaces,
equaling both the electric dipole (ED) and magnetic dipole
researchers have consequently demonstrated diverse applica-
(MD) in the ADHMS,49−54 we realized a full range of the 2π
tions, such as metalenses,13,14,16,18,19,23,24 anomalous refrac-
tion,25−27 holography,28−32 vortex beam generation,33,34 and
quarter-wave plates.35,36 Received: October 27, 2021
In fact, a key to realizing the aforementioned cutting-edge Accepted: December 14, 2021
applications is to offer a full range of 2π phase coverage, which Published: December 27, 2021
is necessary to control the wavefront of the incident light. To
date, there exist four mechanisms to satisfy the demanded 2π
phase coverage, namely, resonating meta-atoms,26,37,38 wave-

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Figure 1. (a) Scheme of all-dielectric Huygens’ metasurface composed of titanium dioxide (TiO2) embedded in glasses. (b) Simulated
transmittance spectrum of the metasurface with a TiO2 diameter of 176 nm. It revealed a near-unity transmittance at a wavelength of 381 nm. The
radiation powers of both electric dipole and magnetic dipole are also included, which concurrently peak at 381 nm, consistent with the wavelength
of the near-unity transmittance. (c) Phase of Huygens’ metasurface with a 2π change around the operating frequency.

Figure 2. (a) Transmittance and phase spectra of Huygens’ metasurface with titanium dioxide (TiO2) diameters of 220 and 120 nm, respectively.
The two shows separated ED and MD and only π change at resonance. We can still obtain near-unity transmittance near the operating frequency.
(b) Transmittance and (c) phase distribution with respect to different TiO2 diameters. At 381 nm, we found that the transmittance approaches
unity and covers the entire 2π phase change.

phase change, transmittance efficiency of 80%, and beam- propagating along the z-direction. The corresponding radiation
bending efficiency of 15%. We believe that the NUV-ADHMS power, transmittance, and phase are presented in Figure 1b,c,
demonstrated here offers a building block to construct flat respectively. By combining the equivalent radiation powers of
electromagnetic devices, including metalenses, holographic ED and MD at a wavelength of 381 nm, we could observe a
devices, and beam deflectors. unity transmittance (Figure 1b) and a 2π phase coverage

■ DESIGN AND SIMULATION

To realize the NUV-ADHMS, the material used here is TiO2
(Figure 1c). Also included in Figure 1b are the calculated
radiation powers from the ED and MD. These two radiation
powers concurrently peak at 381 nm, which is consistent with
owing to its high dielectric constant (εreal ≅ 6) and low loss the wavelength of the near-unity transmittance to validate that
(εimag ≅ 0) within the NUV regime (see Section I in the near-unity transmittance along with a 2π phase change can be
Supporting Information). Next, we used nanodisks as the units realized by simultaneously equaling the excited ED and MD.
of this metasurface owing to their simplicity, insensitivity to Furthermore, we modulated the radius of the TiO 2
polarization, and ease of fabrication. It should be noted that nanodisks to scrutinize the change in transmittance and
these TiO2 nanodisks are hosted on a silica substrate and then phase so as to establish a design guideline for NUV-ADHMS.
covered by a homogeneous silica superstrate (dielectric For example, for the case of D = 220 nm, there exist two
constant = 1.3). Such a symmetric boundary condition can resonance dips at 420 and 396 nm, which correspond to ED
prevent the Fabry−Perot resonance in the glass substrate42 and and MD, respectively, as shown in the lower panel of Figure 2a.
thereby identify the transmission spectrum of the Huygens’ At the resonance states, each dipole provided a phase change
metasurface more clearly. Finally, the NUV-ADHMS com- of the π coverage alone. By scaling down the diameter of TiO2
prised a periodic array of TiO2 nanodisks, with a diameter (D) nanodisks, for instance, D = 120 nm, we can blue-shift the
of 176 nm, periodicity (P) of 240 nm, and height (H) of 80 positions of both ED and MD to shorter wavelengths, as
nm, as presented in Figure 1a. shown in the upper panel of Figure 2a. It should be noted that
The designed NUV-ADHMS was simulated using a finite- in this case, there appears only one broader transmittance dip
element method, a commercial solver (COMSOL Multiphysics centered at 360 nm, neither two dips nor one peak. The reason
5.3a). We set periodic boundary conditions in both the x- and for this broad transmittance dip stems from the partial
y-directions and excited this HMS using plane wave overlapping, not coincidence, of ED and MD. Next, we
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Figure 3. (a) Scheme of the bending device composed of eight meta-atoms with different disk diameters. (b) Simulated electric field distribution of
the beam-bending device. The bending angle is 8.7° in excellent agreement with the analytical calculation.

Table 1. Corresponding Titanium Dioxide Diameters for the Targeted Phase in the Simulation
diameter (nm) 120 150 162 168 172 176 180 186
transmittance (au) 0.98 0.98 0.95 0.89 0.88 0.92 0.90 0.87
phase (°) 176 217 262 305 347 40 86 127

Figure 4. (a) Scanning electron microscopy images of Huygens’ metasurfaces with titanium dioxide diameters of 130, 155, 165, and 190 nm. (b)
Scheme of the optical measurement setup. A laser-driven light source provides a broadband incident light at a wavelength range of 180−2100 nm
for transmittance measurement. On the other hand, a 405 nm laser is used to measure the bending ability of the proposed bending device. (c)
Measured transmittance at the four diameters. Note that ↓ and ↑ with the same color of the curves indicate the locations of ED and MD,
respectively. CCD, charge-coupled device; LDLS, laser-driven light source.

swept the radius of the TiO2 nanodisks to correlate the radius Finally, to demonstrate phase manipulation of the HMS, we
with not only the maximum transmittance but also the desired introduced a beam-bending device as an example. As presented
phase change. The results are presented in Figure 2b,c. For in Figure 3a, one unit of this beam-bending device is
instance, at the specific wavelength of 381 nm (indicated by comprised eight nanodisks, with respective diameters of 120,
150, 162, 168, 172, 176, 180, and 186 nm. Based on the
dashed lines), we offer transmittance near unity for all radii of
previous finding presented in Figure 2, these integrated eight
the nanodisks and specify the desired phase change by
meta-atoms correspond to transmittance/phase changes of
selecting the corresponding radius. Based on this guideline of 0.98/176, 0.98/217, 0.95/262, 0.89/305, 0.88/347, 0.92/40,
coinciding MD and ED, one can design a NUV-ADHMS with 0.90/86, and 0.87/127° in sequence (as tabulated in Table 1)
a near-unity transmittance and full range of 2π phase coverage for the anomalous diffraction. The bending angle follows the
at a specified operation wavelength. generalized boundary condition as presented in eq 138
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i λ yi dϕ y
nt sin(θt ) − ni sin(θi) = jjj zzzjjj zzz
k 2π {k dx {
frequency range of 180−2100 nm, followed by two lenses to
(1) reduce the beam spot. For the beam-bending measurement, we
used a 405 nm laser instead. In both measurements, objective
where nt is the refraction index of the transmitted region, ni, is lens 1 (OB1) focused the incoming light onto the sample,
the refraction index of the incident region, θt is the transmitted objective lens 2 (OB2) collected the transmitted light, and a
angle, θi is the incident angle, ϕ is the τηε phase differences beam splitter bisected the light to charge-coupled device and
among meta-atoms, and x is the periodicity of the meta-atom. spectrometer for imaging and transmittance spectrum,
In the theoretical calculation, the bending angle θt is 8.67° as nt respectively. The measured transmittances of four fabricated
and ni equal to 1.3, θi = 0, ϕ = 45°, and x = 240 nm. To further TiO2 nanodisks are plotted in Figure 4c, and the ED and MD
corroborate the calculation, we conducted the simulation and are indicated by the arrows (i.e., ↓ for ED and ↑ for MD).
recorded its field distribution, as plotted in Figure 3b. From the Along with the increase in the diameter of TiO2 nanodisks, it
field distribution, the bending angle is around 8.7°, which can be clearly observed that both ED and MD not only red-
agrees well with the calculation.

■
shifted to longer wavelengths but also approached each other
and eventually merged together at a diameter of 190 nm. By
FABRICATION AND MEASUREMENT the way, the resonance tail of D = 165 nm is a litter lower
We employed an electron beam lithographic process to define down the transmittance at a wavelength of 420 nm. It should
the pattern of the NUV-ADHMS. First, we spin-coated a be noted that in this case of the so-called Huygens’ condition,
the transmittance of the TiO2 nanodisks reached a maximum
Table 2. Calibrated and Fabricated Diameters of Eight (i.e., 70%) and thus enabled a building block for flat optical
Titanium Dioxide Nanodisks for the All-Dielectric Huygens’ devices with excellent efficiency.
Metasurface at a Near-Ultraviolet Regime Finally, Huygens’ condition appeared at a diameter of 176
and 190 nm for simulated and experimental results,
number of 1 2 3 4 5 6 7 8 respectively. Such a discrepancy might stem from the
nanodisks
calibrated 96 136 148 154 158 162 164 170
fabrication imperfection and mismatched material properties
diameter (the dielectric constants of the glass substrate and the spin-on
fabricated 94 128 147 151 158 164 166 170 glass are 1.44 and 1.45, respectively). Therefore, we calibrated
diameter the dimensions of eight TiO2 nanodisks accordingly (listed in
Table 2) to construct the HMS in the beam-bending
demonstration. The fabricated results are presented in Figure
positive-tone resist, poly(methyl methacrylate), on a preclean 5a, and the recorded imaging of the beam bending is presented
silica substrate with a rotation speed of 3500 rpm, in Figure 5b. From the left to the right, three bright spots
corresponding to a thickness of about 200 nm. Second, a deflected by the fabricated NUV-ADHMS emerged, which
conductive polymer was also spin-coated to the substrate to correspond to the diffraction orders of −1, 0, and 1 with an
suppress the charging effect from the insulating substrate. intensity ratio of 1:10:2. The lower bending efficiency of 15.4%
Third, we used an electron-gun evaporator to deposit a thin- stems from the offset of the operating wavelength due to the
layer TiO2 of 80 nm and then conducted a liftoff process to lack of a 420 nm laser in our measurement setup and the little
complete TiO2 nanodisks. Finally, a spin-on-glass was applied deviation between the designed and fabricated nanodisks’
to the sample to thoroughly cover the nanodisks within a diameters (see Section V in the Supporting Information).
homogeneous environment. Such a symmetric boundary Evidently, the first-order diffraction occurs at the bending
condition could prevent the Fabry−Perot resonance in the angle of 11° at 405 nm, validating the 2π phase coverage
interface between two different materials (i.e., air−glasses through all-dielectric HMSs in the NUV regime.

■
interface) and thereby balance the magnitudes of the excited
ED and MD. The fabricated TiO2 nanodisks with diameters of
130, 155, 165, and 190 nm are presented in Figure 4a, which CONCLUSIONS
slightly deviate from the designed values presented in Figure In this work, we successfully presented an ADHMS to harness
3a. the wavefront at the NUV regime. This NUV-ADHMS fulfills
Next, we measured the transmittance and beam-bending two key requirements of great transmittance and 2π phase
capability of the fabricated NUV-ADHMS. The corresponding coverage. For the former requirement, we used TiO2 because
optical setup is presented in Figure 4b. For the transmittance this dielectric material possesses a great dielectric constant and
measurement, we adopted a laser-driven light source with a a low intrinsic loss at this high-frequency range. For the latter

Figure 5. (a) Scanning electron microscopy images of Huygens’ metasurfaces with gradient diameter. (b) Measured spots deflected by the device
with a diffraction order of −1, 0, and 1, with an intensity ratio of 1:10:2. The deflection angle is 11°.

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requirement, we designed nanodisks as resonators. We work. T.-A.C. and Y.-C.C. performed the fabrication experi-
indicated design guidance for deliberately controlling the ments, sample characterization, calculations, and simulations.
diameters of the TiO2 nanodisks, with which one can excite T.-A.C., Y.-C.C., T.-Y.H., Y.-P.K., Y.-J.L., and T.-J.Y.
both ED and MD in the TiO2 nanodisks to offer the demanded contributed to data analysis and manuscript preparation.
phase changes. As a consequence, this NUV-ADHMS Notes
comprises an array of TiO2 nanodisks with eight different
The authors declare no competing financial interest.

■
diameters to offer the demanded great transmittance and 2π
phase coverage. For example, in the simulation, near-unity
transmittance and the full range of 2π phase coverage at a ACKNOWLEDGMENTS
wavelength of 381 nm are suggested; in the experiment, a This work was supported by grants from the Ministry of
transmittance above 70% at a wavelength of 420 nm appeared. Science and Technology and Academia Sinica. (MOST 107-
The deviation of operation wavelength and efficiency might 2221-E-007-016-003-MY3, MOST 110-2221-E-007-051-MY3,
stem from fabrication imperfection and different material 110A2049EW, 110QR001J4, MOST 106-2112-M-001-036-
properties in the simulation and experiments. Finally, we used MY3, MOST 109-2112-M-001-043-MY3, and AS-CDA-108-
HMS to bend the NUV light at its off-resonance wavelength of M08).

■
405 nm, revealing an 11° bending with an efficiency of 15.4%
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