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Effect of high index sphere size on effective refractive index of random

nanocomposites
To cite this article: Andrey V. Panov 2018 J. Phys.: Conf. Ser. 1092 012110

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METANANO 2018 IOP Publishing
IOP Conf. Series: Journal of Physics: Conf. Series 1092 (2018)
1234567890 ‘’“” 012110 doi:10.1088/1742-6596/1092/1/012110

Effect of high index sphere size on effective refractive index

of random nanocomposites
Andrey V. Panov
Institute of Automation and Control Processes, Far East Branch of Russian Academy of Sciences, 5,
Radio st., Vladivostok, 690041, Russian Federation
E-mail: andrej.panov@gmail.com

Abstract. The linear and nonlinear optical properties of random composites are investigated with the
use of the three-dimensional finite-difference time-domain (FDTD) simulations of light propagation.
An effective linear refractive index of the mixture as a function of the GaP spherical inclusion size is
constructed. This dependence is non-monotonic reaching a maximum just below the first optical resonance.
It is shown that the effective Kerr third-order susceptibility of the nanocomposite grows by orders near the
optical resonance.

The optical resonances of high refractive index nanoparticles have been studied for more than a
century [1]. Recently, particular attention has been given to unusual properties of the high index particle
structures: induced transparency [2], controllable strong anisotropic scattering [3], switchable invisibility
[4]. It was supposed that these particles show enhanced optical nonlinearity due to the field concentration
at the optical resonances [5].
The small dielectric spheres with the high refractive index have certain modes at which optical
resonances are displayed. The resonance inside the particles arises from the self-maintaining oscillations
of the electric and magnetic fields. The magnetic dipole resonance is most pronounced and has the
smallest size of the particle when [6]
nkr = π, (1)
where n is the refractive index inside the sphere, k = 2π/λ are the wavenumber and the wavelength
in vacuum, r is the radius of the sphere. At these resonances, the scattering from the particle has the
Fano profile as a result of the interference between the resonant Mie scattering and the non-resonant
background scattering [5].
The optical properties of the nanoparticle systems are usually treated by effective medium theories,
for example, linear [7, 8] or nonlinear, [9]. In these theories, the effective refractive index of the mixture
containing the inclusions is calculated. Generally, the effective medium theories assume the uniform
field distribution inside inclusions that is nkr  1.
In this work, the effective nonlinear refractive index of the nanocomposite containing identical
spherical inclusions is examined as a function of the particle size by means of the FDTD modeling with
the meep solver [10]. The simulations were conducted for the randomly arranged systems of the particles
with the sizes from small compared with the wavelength to the magnetic dipole resonance radius and
larger. The modeling was done using the method described in Ref. [11]. This method utilizes the phase
change of the Gaussian beam transmitted through the studied sample. This phase change is computed
for different intensities of the Gaussian beam enabling one to estimate the real parts of both the linear

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METANANO 2018 IOP Publishing
IOP Conf. Series: Journal of Physics: Conf. Series 1092 (2018)
1234567890 ‘’“” 012110 doi:10.1088/1742-6596/1092/1/012110

n0 rec
1.5 n0 B
n0 L
1.4

1.3
n0

1.2

1.1

1
20 30 40 50 60 70 80 90
r, nm

Figure 1. Dependence of the effective linear refractive index of the random nanocomposite on the sphere
radius r for a fixed number of the particles (1000). The effective refractive index n0 rec is calculated using
FDTD modeling, n0 B and n0 L are results of the effective medium theories [7, 8].

refractive index and third-order susceptibility of the sample. All the simulations were conducted for the
wavelength of 532 nm.
The studied samples represent the system of the disjoint spheres of the same radius r randomly
arranged in space. Two different arrangements of a thousand of the particles inside the sample were
randomly generated, the size of the spheres was varied for each configuration. The gallium phosphide
(GaP) was selected as a material of the inclusions because of the high value of the real part of linear
refractive index n0 in = 3.49 at λ = 532 nm [12] and moderately low extinction coefficient (0.0026). In
this work, only the real part of the refractive index was used since meep cannot simulate simultaneously
lossy and nonlinear medium. The third-order optical susceptibility of the inclusions χ(3) in
= 2 × 10−10 esu
[13] was applied to the computations.
The size of the computational domain for the FDTD simulations was 4 × 4 × 30 µm with the space
resolution of 5 nm. The size of the sample with the nanoparticles was 4×4×0.8 µm, the distance between
the Gaussian beam source and the studied sample was 0.9 µm. The beam radius w0 at the beam waist
was 1.1 µm.
Fig. 1 depicts the computed values of the linear effective refractive index n0 rec of the samples as a
function of the sphere radius. The error bars show the standard deviations of n0 rec . For comparison,
the curves calculated using effective medium theories [7, 8] are given. It should be underlined that this
effective medium theories are unusable for most range in Fig. 1. Moreover, the approximation in Ref. [8]
is elaborated for the cubic lattice of the spheres. As can be seen from the figure, the dependence of
n0 rec on the sphere size is non-monotonic: n0 rec has a maximum below the magnetic dipole resonance
at r = 76.1 nm (Eq. 1), then it drops and rises again. In particular, for the particles with the sizes under
the first optical resonance, the computed effective refractive index coincides with one predicted by the
Lewin approximation [8].
The results of the calculations of the effective third-order susceptibility χ(3)
rec are presented in Table 1.

2
METANANO 2018 IOP Publishing
IOP Conf. Series: Journal of Physics: Conf. Series 1092 (2018)
1234567890 ‘’“” 012110 doi:10.1088/1742-6596/1092/1/012110

r, nm f, % n0 rec n0 B n0 L χ(3)
rec , esu χ(3)
RZPA , esu
20 0.365 1.00464 ± 0.00002 1.00434 1.00380 (2.0 ± 0.7) × 10−15 1.51 × 10−15
30 1.18 1.01636 ± 0.00008 1.01424 1.01442 (1.0 ± 0.2) × 10−14 5.35 × 10−15
40 2.70 1.0405 ± 0.0002 1.03320 1.03908 (4.4 ± 0.5) × 10−14 1.44 × 10−14
50 5.07 1.0864 ± 0.0005 1.06468 1.08926 (1.13 ± 0.07) × 10−12 3.52 × 10−14
60 8.44 1.174 ± 0.001 1.11336 1.18693 (1.12 ± 0.05) × 10−12 8.63 × 10−14
65 10.5 1.249 ± 0.001 1.14620 1.26733 (2.6 ± 0.2) × 10−11 1.38 × 10−13
70 12.9 1.403 ± 0.004 1.18618 1.38453 (5.0 ± 1.2) × 10−09 2.25 × 10−13
80 18.6 1.180 ± 0.008 1.29352 1.88407 (3.0 ± 1.8) × 10−09 6.47 × 10−13

Table 1. The linear refractive indexes and nonlinear susceptibilities χ(3) of random mixtures
reconstructed with the FDTD modeling and predicted by the effective medium theories for different
radii of spheres r. Here f is the volume fraction (concentration) of inclusions, n0 rec is the reconstructed
linear refractive index, n0 B and n0 L are ones calculated using the Bruggeman [7] and Lewin [8] formulas,
χ(3) (3)
rec is the third-order susceptibility retrieved in this work, χRZPA is calculated using [9].

It was not possible to compute χ(3)eff

for the resonance range owing to large errors. The effective χ(3)
calculated using Ref. [9] shows the largest value among other approximations [11]. It is of great
importance that χ(3)
rec is much larger than the prediction of the nonlinear effective medium theory when
the sphere size approaches the optical resonance. Near the magnetic dipole resonance, χ(3) rec of the
nanocomposite even exceeds the third-order susceptibility of bulk GaP. This is due to the giant field
concentration inside the spheres near the resonance [5].
To sum up, the dependence of the nonlinear refractive index of the random nanocomposite on the
size of the spherical inclusions is investigated numerically. The linear effective refractive index of the
mixture falls at the magnetic dipole resonance. The Kerr third-order susceptibility of the composite
abruptly increases near this resonance.

Acknowledgements
The results were obtained with the use of IACP FEB RAS Shared Resource Center “Far Eastern
Computing Resource” equipment (https://www.cc.dvo.ru). This work was partly supported by “Far East
Program” of FASO Russia (grant No. 18-3-023).
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