ARTICLE

https://doi.org/10.1038/s41467-020-15444-0 OPEN

Infrared dielectric metamaterials from high

refractive index chalcogenides
H. N. S. Krishnamoorthy1,3 ✉, G. Adamo1,3, J. Yin 1, V. Savinov2, N. I. Zheludev1,2 & C. Soci1 ✉

High-index dielectric materials are in great demand for nanophotonic devices and applica-
tions, from ultrathin optical elements to metal-free sub-diffraction light confinement and
1234567890():,;

waveguiding. Here we show that chalcogenide topological insulators are particularly apt
candidates for dielectric nanophotonics architectures in the infrared spectral range, by
reporting metamaterial resonances in chalcogenide crystals sustained well inside the mid-
infrared, choosing Bi2Te3 as case study within this family of materials. Strong resonant
modulation of the incident electromagnetic field is achieved thanks to the exceptionally high
refractive index ranging between 7 and 8 throughout the 2–10 μm region. Analysis of the
complex mode structure in the metamaterial allude to the excitation of circular surface
currents which could open pathways for enhanced light-matter interaction and low-loss
plasmonic configurations by coupling to the spin-polarized topological surface carriers,
thereby providing new opportunities to combine dielectric, plasmonic and magnetic meta-
materials in a single platform.

1 Centre for Disruptive Photonic Technologies, TPI, SPMS, Nanyang Technological University, Singapore 637371, Singapore. 2 Optoelectronics Research

Centre & Centre for Photonic Metamaterials, University of Southampton, London SO17 1BJ, UK. 3These authors contributed equally: H.N.S. Krishnamoorthy,
G. Adamo. ✉email: harish.k@ntu.edu.sg; csoci@ntu.edu.sg

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T
opological insulator (TI) crystals feature time reversal sym- imaginary parts of the calculated complex refractive index
metry-protected, highly conducting surface states character- n ¼ n þ ik). Its dispersion is characterized by contrasting beha-
(e
ized by Dirac dispersion and spin-momentum locking of viors in two regions of the spectrum: (i) the short wavelength
carriers that encapsulate a semi-conducting bulk1–3. They are an (0.25–1.50 μm) region with strong absorption (high k), resulting
extremely attractive class of materials for electronic4, spintronic5 from interband transitions in the bulk, and (ii) the long wave-
and, more recently, photonic6,7 applications, where coupling of light length (~2–16 μm) region featuring strong polarizability (high n).
to the topologically protected surface carriers may lead to propa- Correspondingly, the permittivity is negative throughout the
gating surface plasmon polaritons with very little scattering and 0.25–0.85 μm region (n < k)9,20, where the material is plasmonic.
other exotic phenomena, such as hybridization of spin and surface The typical concentration of surface carriers in these materials
plasmons8. This has motivated extensive studies of electromagnetic (1012–1013 cm−2) results in their contribution to the optical
properties of TI chalcogenide crystals over a broad range of fre- conductivity becoming significant in the long wavelength region
quencies from THz to UV9–15. Interaction of electromagnetic waves above 6 μm20, as manifested by a small decrease of the refractive
with the topological surface states can be enhanced by suitably index.
structuring the TI crystals with subwavelength units, such as reso- Spectroscopic studies were carried out on exfoliated films of TI
nant metamolecules, giving rise to absorption and localization of single crystal samples of Bi2Te3 with thickness ranging from 10 to
the electromagnetic field9,16. TI metamaterials have been realized at 100 μm. We characterized optical properties over a broad spectral
THz and UV–visible frequencies, where the material response is range, from the UV to the mid-infrared by means of variable angle
more plasmonic due to free surface carriers and bound bulk car- ellipsometry (in the UV to near-infrared range) and near-infrared
riers, respectively9,16–18. However, there have been hardly any to mid-infrared reflection measurements, from which we extracted
studies on resonant TI structures at intermediate near-infrared and the experimental complex refractive index dispersion (Fig. 2b).
mid-infrared frequencies, where the compositionally tunable The experimental dispersion compares well with the calculated
refractive index is extremely high19, and optical conductivity from one, showing absorption and negative permittivity at the shorter
charge carriers in topological surface states becomes significant20. wavelengths, and strong dielectric behavior in the infrared.
Within the family of chalcogenide crystals, we select Bi2Te3 to The deviation from the calculated dispersion at longer
demonstrate dielectric metamaterial structures in the technologi- wavelengths is due to a sharp decrease of the refractive index
cally important near to mid-infrared frequency window. Bi2Te3 has and an increase of the extinction coefficient induced by free bulk
a refractive index between 7 and 8 over the 2–10 μm spectral range, carriers from intrinsic doping. This effectively creates a third
which is much larger than typical infrared dielectric materials, such region of high refractive index and low losses between 7 and 10
as Si (n = 3.44)21, Ge (n = 4.07)22, PbTe (n = 5.61)23, and GST μm for the crystals in our hands. The dashed lines in Fig. 2b show
(n = 6–7.2)24. the experimental optical constants after removing the bulk Drude
Here we show that the high refractive index of the chalcogenide contribution for comparison with the DFT calculation results,
crystals can be used to generate strong infrared resonances and showing fairly good agreement between the two once the intrinsic
associated complex mode structures with surface circular cur- doping contribution is excluded.
rents, opening up new opportunities to couple light with spin-
polarized topological surface state carriers. Broadly tunable infrared dielectric metamaterials. Optical
materials with high refractive index and low losses such as Bi2Te3
in the mid-infrared are in great demand for dielectric metama-
Results terials, as they can produce strong mode confinement and narrow
The high infrared refractive index of TIs. We started by carrying resonances for small form factor devices30. On this premise, we
out first-principles calculations and spectroscopic measurements fabricated infrared nanoslit arrays via focused ion beam milling
of single crystal Bi2Te3. Density functional theory (DFT) calcula- on the surface of exfoliated Bi2Te3 crystals. The slit array geo-
tions based on the local density approximation (LDA) were metry was chosen for geometrical simplicity and designed to have
employed to study the electronic band structures and optical pronounced resonances across the entire infrared spectrum by
properties of the rhombohedral-phase Bi2Te3 (see the crystal varying the nanoslit length (L) from 1.0 to 4.3 μm. Representative
structure in Fig. 1a) using the Quantum ESPRESSO (QE) pack- top-view and cross-sectional SEM images of the fabricated
age25. Experimental lattice parameters of bulk Bi2Te326,27 were nanoslit arrays are shown in Fig. 3a–d. Infrared microscopy
used to build the initial structure, and ground states geometry of reflection measurements were carried out with incident electric
the Bi2Te3 crystals was obtained by the total energy minimization field vector polarized both parallel (REk ) and perpendicular (RE⊥)
method upon relaxing their crystal framework and atomic coor-
to the length of the slits. The slit arrays show resonant response
dinates. We calculated the band structure of Bi2Te3 with and
only when excited with perpendicular polarization. To highlight
without spin–orbit coupling (SOC). Due to the presence of heavy
these resonances, we plot the reflection spectra in a differential
elements such as Bi and Te, relativistic effects and SOC have
form, ðRE?  REk Þ=REk , for the various slit lengths (Fig. 3e). Two
significant impact on the band structure. Without SOC, the bands
have the typical parabolic dispersion with a direct gap at the Γ distinct resonances are clearly observed in the plot, the funda-
point. However, the presence of SOC leads to band-inversion at mental resonances (indicated by ▼) and, the second-order
the Γ point and a topologically non-trivial gap is induced (Fig. 1b resonances (indicated by ▽) which appear in the measured
top panel) with the Dirac dispersion appearing in the case of a thin spectral region for slits longer than 1.5 μm. Figure 3f shows the
slab (Fig. 1b bottom panel). The optical response was calculated by variation of the resonant wavelength as a function of slit length,
employing the Bethe–Salpeter equations (BSE) method with the clearly indicating a linear spectral red-shift with scaling factors of
YAMBO code, using ground-state wavefunctions from QE 2 and 1 times the slit length for the fundamental and second-
package28,29. The imaginary part of the permittivity was deter- order resonances, respectively31.
mined by evaluating direct electronic transitions between occupied
and higher-energy unoccupied electronic states and the real part Nature of resonant modes and circular surface currents. To
was obtained by employing Kramers–Kroning transformation on further our understanding of the nature of the main resonant
the imaginary part. Additional details on optical response calcu- mode, we carried out finite-element method (FEM) simulations
lations can be found in ref. 20. Figure 2a shows the real and of the nanoslit array, over the corresponding wavelength interval.

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a b
LDA LDA+SOC
1.0

0.5
bulk
0.0

–0.5

Energy (eV)
–1.0
Γ Z F Γ L
0.50 Surface Brillouin Zone

Γ K M
0.25
Z
F

Γ K
slab
0.00 L
Brillouin Zone

Bi/Sb –0.25
Se/Te
–0.50
K Γ M

Fig. 1 Topological insulator properties of Bi2Te3. a Crystal structure of rhombohedral-phase Bi2Te3. b Band structure of Bi2Te3 bulk (top panel) and slab
(bottom panel) calculated at the LDA level, with (red lines) and without (blue lines) spin–orbit coupling. Including the latter leads to band-inversion at the Γ
point and gives rise to topologically protected states at the surface (bottom panel). Inset of the bottom panel shows Brillouin zone of the crystal indicating
the main symmetry points.

a b
Calculated Measured
8 8
Optical constants

Optical constants

6 6
n Actual w/o Bulk Drude
4 k 4 n n'
k k'

2 2

0 0
2 4 6 8 10 12 14 16 2 4 6 8 10 12 14 16
Wavelength (μm) Wavelength (μm)

Fig. 2 Infrared refractive index of Bi2Te3 topological insulator crystals. Dispersion of the complex refractive index a calculated from first-principles
technique and, b measured experimentally (solid lines) from ellipsometry and infrared spectroscopy measurements. The dashed lines correspond to the
case in which the Drude contribution from bulk free carriers is removed.

Figure 4a compares the experimental and simulated differential dipole (order 0), magnetic dipole and electric quadrupole (order
reflection spectra of the longest slit (L = 4.3 μm) arrays, showing 1), toroidal dipole, magnetic dipole, and electric quadrupole
good agreement between the two. Corresponding maps of the (order 2), etc., depicted schematically in Fig. 4g. Noteworthy is
resonant electric and magnetic fields at 8.55 μm are plotted in the fact that toroidal-like field configurations can be generated in
Fig. 4b, c for incident electric field polarization perpendicular to the presence of multiple modes. The differential reflection
the slits. The field-maps for the minor mode at 4.35 μm are spectrum calculated from multipole analysis is shown as dashed
plotted in Fig. 4d, e. Contrary to conventional expectations, a lines in Fig. 4a and agrees fairly well with the simulated and
circulating pattern for the magnetic field as displayed by the experimental spectra. For more details of the multipole analysis,
mode at 8.55 μm (Fig. 4b, c), does not necessarily imply that the refer to Supplementary Note 1. The multipole contribution
resonance is a toroidal dipole. The exact multipole decomposi- for incident non-resonant polarization (electric field parallel
tion, shown in Fig. 4f, shows that the situation is far more to the slit length) is shown in Supplementary Fig. 2. We note that
nuanced: the plot of the multipole components expressed in the overall reflection response of the slit arrays depends on the
terms of the current density (see Supplementary Eq. (12)) shows interference of the various multipoles based on their amplitude
that the metamaterial excitation is not dominated by a particular and phases which is rather complicated and can be illustrated
mode, but is a combination of multiple modes, such as the electric with the aid of phasor diagrams (Supplementary Note 3). We also

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a c e 0.00 0.00

–0.15 –0.15
L = 2.0 µm unstructured

0.00 0.00

–0.15 –0.15
L = 1.8 µm L = 4.3 µm
b d

Differential reflection
0.00 0.00

–0.15 –0.15
L = 1.6 µm L = 3.7 µm

0.00 0.00
f –0.15 –0.15
Resonant wavelength (µm)

L = 1.4 µm L = 3.2 µm
8 1st order resonance
2st order resonance
7 0.00 0.00

6 –0.15 –0.15
L = 1.2 µm L = 2.8 µm
5
0.00 0.00
4
3 –0.15 –0.15
L = 1.0 µm L = 2.2 µm
2
5 10 15 5 10 15
1.0 1.5 2.0 2.5 3.0 3.5 4.0 Wavelength (µm) Wavelength (µm)
Slit length (µm)

Fig. 3 Infrared resonances of nanoslit metamaterials. a–c SEM images of slit arrays with lengths L = 1.0, 2.0, and 4.3 μm, respectively. Scale bar
corresponds to 4 μm. d Cross-sectional image of slit array of length 4.3 μm. Scale bar corresponds to 2 μm. Dashed light yellow lines are an aid to mark the
v-shaped contour of the slit. e Experimental infrared differential reflection spectra from slit arrays of different slit lengths from 1.0 to 4.3 μm. Pronounced
resonances, both first (▼) and second order (▽) are observed that red-shift with the slit length. f Resonant wavelength as a function of slit length for the
fundamental and second order resonant modes in the nanoslit arrays.

–0.06 a b c
Differential reflection

–0.12
E H

–0.18
d e
measured
simulated- COMSOL
–0.24 calculated - multipole analysis

Order 0
3.00 f Order 1 E H
Order 2
Order 3
Multipole contribution

Order 4

2.00
g

1.00

0.00
4 6 8 10 12
Wavelength (μm) Order 0 Order 1 Order 2

Fig. 4 Field maps and complex mode structure. a Experimental (solid blue), simulated (solid dark cyan) and calculated (dashed lines) differential
reflection spectra of Bi2Te3 metamaterial slit array of length 4.30 μm. The fundamental and second-order resonances at 8.55 and 4.35 μm, respectively, are
evident in the plot. The sharp peaks in the simulated and calculated spectra around 4.60 and 6.50 μm are due to diffraction effects. Maps of electric (E)
and, magnetic (H) fields determined by FEM simulations showing the nature of the mode at the, b, c fundamental, and d, e second-order resonances. The
maps have been calculated over one half of the slit, for simulation size purposes. The cyan outline overlaid on the color maps indicates the full slit and
simulation region for clarity. f The contribution of various multipoles to the (displacement) current excitation induced in the metamaterial by the incident
wave polarized perpendicular to the slits, including electric dipole (order 0), magnetic dipole (order 1), electric quadrupole (order 1), and toroidal dipole
(order 2). g Schematic representation of the various modes in the metamaterial. See Supplementary Note 1 for further details.

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Table 1 Optical response function model.

Oscillator Formula Fitted parameters (cm−1)

Tauc–Lorentz Aω γðωω Þ
2   ω0 = 10,902
ε2 ¼ ω1 0 2 2 g2 Θ ω  ωg
ðω ω0 Þ ωg = 1300
R 0 ω0 Þdω0
1
ε1 ¼ 1 þ π2 ω ωε202ðω 2
A = 7.69e5
0 γ = 12,229
ω2p
Lorentz εðωÞ ¼ ε1 þ ω2 ω2 iγω ε1 ¼ 1; ω0 = 4343.7
0
ωp = 19,088; γ = 3625.4
ω2
Drude εðωÞ ¼ ε1 þ ω2 ω2p iγω ε1 ¼ 1; ω0 = 0
0
ωp = 3147.5; γ = 165.6

Parameters of the oscillators used to model the dielectric function of Bi2Te3 crystals throughout the optical spectral range.

note that the minor mode at 4.35 μm also shows similar behavior unstructured TIs crystals and microscopy reflection spectra of structured Bi2Te3
with circulating magnetic fields but with two vortices indicating were measured using a Bruker Hyperion microscope coupled to a Bruker Vertex
80v spectrometer. Spectroscopic ellipsometry data were collected using a J.A.
that it is a second-order mode. Supplementary Movies 1–4 show Woollam VASE ellipsometer in the 250–1650 nm spectral range over three angles
the evolution of the electric and magnetic fields within the of incidence (30°, 50°, and 70°), and analyzed using the CompleteEASE ellipso-
metamaterial over half a cycle (0–π) of the phase. metry data analysis program. The refractive index values in the infrared were
determined using the experimentally measured near-to-mid-infrared reflection
spectrum and the dielectric constants in the UV–near infrared range measured
Discussion from ellipsometry. This analysis was carried out using the RefFIT program wherein
The high-order modes supported by metamaterials32–34 enable a combination of Tauc–Lorentz, Lorentz, and Drude oscillators were used to model
strong light localization and confinement, which may be suitable simultaneously, the ellipsometric dielectric constants as well as the infrared
reflection spectrum, from which the refractive index of the material in the infrared
for applications in nonlinear and laser optics35,36, or in coupling spectral range was determined. In the Reffit program, the infrared reflection
to high-order transitions in atoms or molecules. In the context of response was modeled using the model ‘Reflectivity of a Film (Epsilon + Mu) on a
TI metamaterials, the unique nature of the resonant fields fea- Substrate (code = −18)’. The parameters of the oscillators describing the material
turing circular currents on the surface of the TI may be exploited optical function are shown in Table 1.
to couple light with spin-polarized carriers and gain optical access
to the topological surface states that encapsulate the material Simulations. The optical response of the nanoslit array was simulated using full-
wave Maxwell equations solver COMSOL45. The simulations were carried out for a
conformally37. This becomes particularly relevant in the mid-IR 3D structure using perfect electric/magnetic conductor boundary conditions on the
region, where chalcogenide crystals feature a combination of high mirror symmetry plane containing the long axis of the slit for electric field
refractive index and larger contribution of topological surface polarized perpendicular/parallel to the slit. In the multipole analysis, the number of
states to the optical conductivity. higher-order modes obtained is dependent on the position of the air–metamaterial
interface relative to the z = 0 plane. The optimal position of this interface is chosen
Overall, the TI chalcogenide crystal family is an exceptionally such that the differential reflection as well as the field induced in the metamaterial
versatile material platform for infrared applications based on can be quantified with the minimum possible number of modes (in this case 5),
high-index, low-loss dielectric metamaterial architectures38, and corresponds to z = −1200 nm for the mode contributions shown in Fig. 4f.
including ultrathin flat optical elements39, sub-diffraction light
confinement and waveguiding40, and nonlinear optics41. Low-loss Data availability
mid-IR metamaterials are also highly sought for enhanced sen- Following a period of embargo, the data from this paper can be obtained from the
sing of molecular fingerprints based on strong light University of Southampton ePrints research repository, https://doi.org/10.5258/SOTON/
D1252.
confinement42,43. Chalcogenide crystal metamaterials add
broadband tunability of the resonances by compositional44 and
structural design to the high refractive index. Moreover, as shown Code availability
Following a period of embargo, the codes used in this paper can be obtained from the
here for Bi2Te3, the inverse geometry of nanoslits carved in high- University of Southampton ePrints research repository, https://doi.org/10.5258/SOTON/
index crystals induces higher-order complex modes outside the D1252.
dielectric medium, which provide additional pathways to sense
changes in the surrounding environment. Received: 24 October 2019; Accepted: 28 February 2020;
In conclusion, chalcogenide TI crystals are a compelling
materials platform for photonic applications in the infrared part
of the spectrum. We have shown that Bi2Te3 exhibits a strong
polarizability with refractive index that exceeds 7 in the 2–10 μm
range, larger than conventional dielectric materials that aids
strong nanostructure resonances sustained deep into the mid- References
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