Nonlocal Response of Polar Nanostructures

Christopher R. Gubbin and Simone De Liberato∗

School of Physics and Astronomy, University of Southampton, Southampton, SO17 1BJ, United Kingdom

Polar dielectric nanoresonators can support hybrid photon-phonon modes termed surface phonon
polaritons with lengthscales below the diffraction limit. In the deep sub-wavelength regime the
optical response of these systems was recently shown to diverge from that predicted through a
standard dielectric description. Recently we developed an analytical, dielectric approach and applied
it to spheres and planar heterostructures, reproducing anomalous features observed in experiment
and microscopic calculations. In this Letter we develop tools to describe the nonlocal response
of polar nanoresonators of arbitrary symmetry. Their validity is verified by comparison to our
arXiv:2006.05208v1 [cond-mat.mes-hall] 9 Jun 2020

previous analytical work, before application to new systems. We show that nonlocal energy transfer
into matter-like modes in the dielectric diminish field enhancement in nanoscale dimers and that
strong nonlocal frequency shifts are possible in macroscopic systems comprised of nanoscopic layers.

Nanophotonics is concerned with concentration and alytical models are tractable in systems with strong sym-
control of light on deep-subwavelength scales. This is metry but cannot be easily generalised beyond this.
possible by exploiting kinetic motion of charged parti- In this Letter we develop new numerical tools to describe
cles, allowing the diffraction limit to be beaten many the nonlocal response of polar nanosystems with arbi-
times over [1]. This is the basis for polar nanophotonics, trary geometry. This is achieved through integration of
where photons are hybridised with the optic phonons of our nonlocal response theory with a commercial finite el-
a crystal lattice in modes termed surface phonon polari- ement solver, the model is distributed for the use of the
tons [2–4]. These modes are highly tuneable [5–9] and community [23]. The approach is validated by compari-
have broad applications in nonlinear optics [10, 11] and son to our previous analytical nonlocal scattering spectra
the fabrication of nanophotonic circuitry [12–14]. for 3C-SiC spheres [22]. The model is then applied to
A key benefit of localised surface phonon resonances the study of spherical dimers, demonstrating the effect
(LSPhRs) is their strong morphological dependance. In of nonlocality on field confinement. Finally we study the
geometries containing sharp corners, or small gaps this nonlocal response of macroscopic resonators containing
results in a dramatic increase in local energy density nanoscale layers, demonstrating the effect of nonlocality
which can be used for sensing applications [15]. When the in a crystal hybrid resonator.
confinement length approaches the atomic length scale Our polar crystal is treated in the continuum limit as
the finite wavelength of the longitudinal optic (LO) and an isotropic lattice with a single phonon branch charac-
transverse optic (TO) phonons becomes important. LO terised by zone-centre longitudinal (transverse) phonon
modes act to push screening charges induced as the parti- frequencies ωL (ωT ) in a quadratic dispersion approxi-
cle boundary into the interior. This leads to a divergence mation analogous to that used in nonlocal plasmonics
from local theories of dielectric response, which assume [16]. Phonons couple to driving electric field E as
screening charges are exactly localised at the scatterer  2  µ
boundary. The nonlocal regime has been studied in plas- ωT − ω (ω + iγ) X + ∇ · τ − E = 0, (1)
monic systems, where excitation of strongly evanescent ρ
bulk plasma waves leads to a charge smearing which lim- in which X is the relative ionic displacement, γ is the
its maximal field enhancement and leads to blue shifted damping rate and ρ and µ are effective mass and charge
modal frequencies [16, 17]. densities. The matrix τ describes the phonon dispersion,
The nonlocal regime is difficult to access, requiring fabri- acting as an effective stress tensor [22, 24] given for an
cation of nanoscale resonators or gaps [18]. It is however isotropic lattice by
expected to be of particular interest for phonon polari-
tons in the field of crystal hybrids, which are constructed
 
2 T
∇X + (∇X) + βL2 − 2βT 2


τ = βT ∇ · XĪ, (2)
from many alternating nanoscale layers of different polar
dielectric materials. In these systems recent studies have
where βT (βL ) are phenomenological velocities describing
shown strong divergence from the local optical response
transverse (longitudinal) phonon dispersion. The model
[19]. These effects can be modelled using a first-principles
is completed by the constitutive relation
method such as density functional theory, [20, 21] how-
ever these methods scale badly to realistic devices with P = µX + 0 (∞ − 1) E, (3)
large numbers of degrees of freedom. To provide more
agile methods we recently developed an analytical con- where ∞ is the high-frequency permittivity and the ma-
tinuum model, describing polar nonlocality in terms of terial polarisation is P.
macroscopic fields [22]. As in local scattering theory an- In a previous publication we solved Eq. 1 and Maxwell’s
 2

equations analytically in simple systems. In principle 0.16

a)
150 Radius 3nm, Local
they could be solved self-consistently by any numerical Radius 2nm

Electric Field
method. Here we employ a method which permits easy 0.14 Radius 3nm
non-uniform meshing as oscillations induced by Eq. 1 oc- Radius 4nm

cur on the nanometer scale, while the wavelength of mid- 0.12

infrared photons is typically 4 orders of magnitude larger.
0
Non-uniform meshing is simple using commercial finite

Extinction Efficiency
0.10
element (FEM) solvers. To use Eq. 1 in a FEM calcu-
lation it must be translated into weak form. The strong
statement is that the left-hand side of Eq. 1 is zero ev- 0.08

erywhere. The corresponding weak statement is that it,

integrated over the computational domain and multiplied 0.06
by a family of test functions Φ, is zero. Integrating by
parts over the computational domain yields 0.04
Z 
µ
d3 r 2
ωT − ω (ω + iγ) 0.02

× βL2 (∇ · X) (∇ · Φ) − βT2


(∇ × X) · (∇ × Φ)
 0.00
b)
+ αX · Φ + 0 (LRA (ω) − ∞ ) E · Φ = 0, (4) Parallel Displacement
Normal Stress
0.14 Shear Stress
where we simplified using the local dielectric function LO Only

0.12
α2 /0 ∞ ρ
 
LRA (ω) = ∞ 1 + 2 . (5)
ωT − ω (ω + iγ)
Extinction Efficiency

0.10

In coupling Eq. 4 with Maxwell’s equations we introduce

the macroscopic fields, X and τ . This means the 0.08

Maxwell boundary conditions are insufficient to deter-

mine mode amplitudes in each layer. The appropriate 0.06
boundary conditions can be derived considering energy
transport across a material interface [22, 25], these are 0.04
continuity of the normal and in-plane ionic displacement
X and of the normal and shear components of the
0.02
effective stress τ · n̂. At interfaces between local and
nonlocal layers the appropriate combination of boundary
conditions has been the subject of active debate [26–28]. 900 910 920 930 940 950 960
It is necessary to apply two of the four conditions, Wavenumber (cm−1 )
leaving a discontinuity in the remaining components.
In plasmonic nonlocality the surface normal current FIG. 1: a) Numerical and analytical extinction cross sections
is constrained [16, 17, 29], we follow that convention for spheres of radius r = 4, 3, 2nm. The numerical results
here by fixing the normal displacement. The second are shown by solid lines. All analytical results are shown by
additional condition is addressed later in this Letter. black dashed lines. The local result is also shown for r = 3nm.
To verify our model we study a system whose nonlocal Inset shows the nonlocal electric field magnitude for r = 4nm.
b) Comparison of numerical extinction cross sections using
response is analytically calculable. We demonstrated
various additional boundary conditions for r = 4nm.
that nonlocal extinction spectra of nanoscopic 3C-SiC
spheres are well described by a quasistatic model in
which the transverse dispersion is neglected and only
the boundary condition on the normal displacement at the Fröhlich frequency, ωF ≈ 933cm−1 , illustrated for
is enforced [22, 29]. This is a reasonable approxima- r = 3nm by the red curve. In the nonlocal case addi-
tion near the Fröhlich resonance where the transverse tional peaks appear in the extinction spectrum. These
phonon is strongly evanescent. Considering the case correspond to quantized LO phonon modes. Eventually
βL = 15.39 × 105 cm s−1 [30] we calculate nonlocal the Fröhlich resonance red shifts as a result of an increase
extinction efficiencies. in the effective nonlocal dielectric function. Note that
Results are shown in Fig. 1a for radius r = 2, 3, 4nm. In in Fig. 1a analytical (numerical) results are illustrated
the local case small spheres exhibit a single resonance by solid (dashed) lines, overlap is exact on this scale
 3

0.12
demonstrating the accuracy of our implementation. The a)
Nonlocal
inset shows the nonlocal electric field magnitude for the Local
4nm sphere, the short wavelength LO phonon oscillation 120
0.10
is clearly visible.
Eq. 1 is a continuum approximation, treating the phonon 100
dispersion phenomenologically through effective stress 0.08
tensor Eq. 2. Phonon dispersions are assumed quadratic,

Extinction Efficiency

Field Enhancement
meaning LO and TO dispersion relations have solutions 80

at all frequencies. In reality the granular structure 0.06

of the lattice prevents this, resulting in a decrease in 60
group velocity to zero at the Brillouin zone edge [31]. In
3C-SiC TO dispersion is weak, meaning that using finite 0.04
βT should not alter the extinction cross-section. 40

We study this in Fig. 1b for a r = 4nm and

βT = 9.15 × 105 cm s−1 [30], for each of the three 0.02
20
secondary boundary conditions. Results are shown in
Fig. 1b. Results constraining shear or normal compo-
nents of τ overlap with the βT ≈ 0 cm s−1 limit explored 890 900 910 920 930 940 950 960
in the prior section, while that constraining the in-plane Wavenumber (cm−1 )

displacement is shifted to the red. For this reason we b)

Nonlocal
constrain the normal stress at the scatterer boundary. Local
120

We have applied our numerical model to systems with Local Nonlocal

analytical solutions, demonstrating its reliability. In the 100
remainder of this Letter we apply it to nanophotonic
systems relevant for modern surface phonon polaritons
Field Enhancement

[6, 32], where lack of symmetry prevents analytical 80

solutions. Firstly we study the effect of nonlocality on

field hotspots, predicted in plasmonic systems to result 60
in strong charge smearing and a corresponding decrease 0 Electric Field 1 0 Electric Field 1

in the maximal field [33]. We consider a spherical dimer,

consisting of two 3C-SiC spheres of radius r = 5nm, 40

separated by a gap of width d. For large gaps the

system modes are those of the isolated spheres studied 20
in Fig. 1. For small d these hybridise into bonding
and antibonding resonances [34], as shown in the local
scattering spectra for d = 2nm in Fig. 2a at 918cm−1 0
0 2 4 6 8 10 12 14 16 18
and 935cm−1 respectively. In the nonlocal spectra (solid Dimer Gap (nm)

line) these modes are supplemented by the longitudinal

modes supported by the dimer, as in Fig. 1a. FIG. 2: a) Comparison of local (red lines) and nonlocal
The antibonding mode is of most interest as opposing (blue lines) extinction efficiencies (solid lines) and field en-
charges enclosing the gap result in strong capacitative hancements (dashed lines) at gap centre and for a dimer pa-
rameterised by sphere radius r = 5nm and intersphere gap
field enhancement. This is demonstrated in the local d = 2nm. b) Comparison of nonlocal (red squares) and local
case by the dashed line in Fig. 2a, which shows field (blue spheres) gap centre field enhancements for a dimer of
enhancement at gap centre. On resonance in the local sphere radius r = 5nm as a function of gap width. Lines are
case this peaks at around 125. In the nonlocal case provided as a guide to the eye. Inset shows the electric field
the enhancement diminishes to around 40. This can be magnitude of the antibonding resonance for d = 1nm.
understood from the field intensity plots inset in Fig. 2b.
In the local case field is strongly localised in the gap,
and is efficiently screened from the sphere interior. In nonlocal case this is offset by increased energy transfer
the nonlocal case screening is less efficient and induced to propagative LO modes in the nanosphere.
screening charges smear into the spheres, diminishing We have discussed nonlocality in systems of nanoscopic
capacitative charging of the dimer. Gap-dependance dimensions or with nanoscale air gaps. Fabrication
is demonstrated in Fig. 2b, where we plot peak field of polar resonators on this scale is challenging, how-
enhancement for the antibonding mode. In the local ever making macroscopic heterostructures containing
case field enhancement diverges as d → 0, while in the nanolayers is a well established process. It was recently
 4

a) suggested that in bulk polar superlattices, termed

Local Nonlocal
3C-SiC r 3C-SiC crystal hybrids [19], a nonlocal description of the
optical response is necessary [22]. Describing a system
SiC

AlN h d AlN
containing many polar layers is beyond the scope of this
AlN
work, however we demonstrate the effect of nonlocality
SiC
in larger resonators containing a small number of
3C-SiC Vacuum 3C-SiC Vacuum nanoscopic polar layers.
0 Electric Field 1 0 Electric Field 1
We apply our model to a typical polar resonator,
b)
0.14
a 3C-SiC nanopillar of height h = 250nm and ra-
1nm Film, Nonlocal
1nm Film, Local
dius r = 500nm on same material substrate [6, 32].
0.5nm Film, Nonlocal We consider a single AlN layer in the pillar cen-
0.12 0.5nm Film, Local tre as illustrated in Fig. 3a, parameterised by
βT = 1 × 105 cm s−1 , βL = 5.1 × 105 cm s−1 [22].
In the dashed lines of Fig. 3b we show the local ex-
0.10
tinction cross section for film thicknesses d = 0.5, 1nm.
Extinction Efficiency

The spectrum shows three features. The first, closely

0.08 resonant with the zone-centre LO phonon in the AlN
(ωL ≈ 887cm−1 , marked by the vertical dashed line) is
the Berreman mode of the AlN film [7], independent of
0.06
the pillar dimensions. Other peaks are photonic modes
resulting from hybridisation of the monopolar mode of
0.04 the nanopillar [6] with the epsilon-near-zero response of
the AlN [7]. In the 1nm case these are more strongly
split around ωL as the increased film thickness results in
0.02
enhanced pillar-film coupling. In the nonlocal case (solid
lines in Fig. 3b) both photonic modes are red shifted,
c) 0.14
this is particularly true for the low frequency mode. The
0.5nm Film, Nonlocal red shift is more pronounced for the 0.5nm film. This
0.5nm Film, Local
0.5nm Bilayer, Nonlocal is because the AlN film supports quantised Fabry-Pérot
0.12 0.5nm Bilayer, Local LO phonon modes which red shift as d → 0, resulting in
a red shift of the hybridised resonances.
Crystal hybrids are comprised not of a single nanoscopic
0.10
layer embedded in bulk but of many such layers [19]. To
Extinction Efficiency

demonstrate how these results of can be extrapolated to

0.08 such systems we consider the effect of adding a second
0.5nm AlN film, separated from the first by a 0.5nm
3C-SiC spacer layer, results are shown in Fig. 3c. In
0.06
the local (dashed lines) cases the additional layer results
in an increased splitting of the photonic modes around
0.04 ωL as a result of increased coupling between the AlN
epsilon-near-zero mode and the pillar resonance. In the
nonlocal case the same thing happens around ω1 . A full
0.02
crystal hybrid would exhibit even larger coupling. Also
shown in Fig. 3a are the electric field magnitude at the
nanopillar boundary in for a 1nm AlN film, normalised
860 870 880 890 900 910
Wavenumber (cm−1 )
to the field maximum in each case. In the local case the
field is localised at the pillar edge. In the nonlocal case
FIG. 3: a) Electric field intensity at the nanopillar boundary.
energy is transferred into the quantised LO mode, with
b) Comparison of local (dashed lines) and nonlocal (solid line) a node at the film centre.
extinction efficiencies for a 3C-SiC nanopillar of height 250nm
and diameter 500nm on deep 3C-SiC substrate containing a We presented a numerical method to study the nonlo-
thin AlN film of thickness 0.5 and 1nm. c) Comparison of local cal response of nanoscopic polar resonators. This extends
(dashed lines) and nonlocal (solid line) extinction efficiencies
previous analytical studies, generalising them to study
for a 3C-SiC nanopillar of height 250nm and diameter 500nm
on deep 3C-SiC substrate containing one and two thin AlN resonators of arbitrary geometry. Furthermore our work
films of thickness 0.5nm on macroscopic nanopillars can be easily extrapolated to
describe the optical response of a crystal hybrid nanopil-
 5

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Corresponding author: [email protected]
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