Radiative Heat Transfer Between Core-Shell Nanoparticles

Moladad Nikbakht
Department of Physics, University of Zanjan, Zanjan, Iran
(Dated: October 24, 2017)
Radiative heat transfer in systems with core-shell nanoparticles may exhibit not only a combi-
nation of disparate physical properties of its components but also further enhanced properties that
arise from the synergistic properties of the core and shell components. We study the thermal con-
ductance between two core-shell nanoparticles (CSNPs). We predict that the radiative heat transfer
in a dimer of Au@SiO2 CSNPs (i.e., silica-coated gold nanoparticles) could be enhanced several
arXiv:1710.07697v1 [physics.app-ph] 20 Oct 2017

order of magnitude compared to bare Au nanoparticles. However, the reduction of several order of
magnitude in the heat transfer is possible between SiO2 @Au CSNPs (i.e., silica as a core and gold
as a shell) than that of uncoated SiO2 nanoparticles.

Radiative heat transfer between objects is sensitively

dependent upon their separation distance. If the sep-
aration is too small compared to the thermal wave-
length, then energy transfer exceeds the well known
classical Plancks law of the black-body radiation1 . In
addition to the separation distance, the radiative heat
transfer in a dimer of nanoparticles depends on vari-
ous properties of the constituent nanoparticles, includ-
ing material composition2,3 , size4 , shape57 , and relative
orientation810 . The proper choice of each of these quan-
tities depends on the desired application which could
include reducing, increasing or rectifying the radiative
heat transfer. In spite of major efforts, manipulating the
radiative transfer in two-body systems by these param-
eters usually does not lead to a drastic change in the
heat transfer. This is an exciting time for nanofluidic
and energy harvesting applications, to manage the ther-
mal flux by nanoparticles. For such applications, novel
ways for tuning the rate of energy transfer is important,
and a unique method for this idea is through the use of
core-shell nanoparticles (CSNPs). Core-shell nanoparti-
cles have received increasing attention since Halas and
co-workers11. During the last decade, a variety of ap-
proaches have been developed for the synthesis of CSNPs,
which provide us with metallic (or dielectric) nanoparti-
cles coated of a shell with a different composition (e.g.,
Au on SiO2 or SiO2 on Au). Several approaches to fab-
rication of CSNPs based on the silica core and gold shell
or gold core and silica shell have been reported1219 . It
is shown by several groups that CSNPs exhibit unique
optical properties which can not be obtained by tradi-
tional nanoparticles with uniform structure2022 . With
the use of core-shell spherical nanoparticles, one has two
dielectric functions, the core radius and the shell thick-
ness as parameters, instead of the single dielectric func-
tion and size as tuning parameters for a bare nanoparti-
cle. An example that can illustrate the significance of
the study of radiative transfer between CSNPs is the
emulsion of metal nanoparticles in an aqueous solution.
Due to the chemical interaction at the surface of the
nanoparticles, interface between nanoparticles and solu-
tion can be viewed as a double layer, suggesting that
such nanoparticles can be modeled by CSNPs. Moreover,
growing interest of researchers in the measuring thermal
Figure 1. Scheme of the system of CSNPs under study. Sys-
tem consists of two identical core-shell nanoparticles with sep-
aration d. Each nanoparticle characterized by its core radius
Rin , outer radius Rout , shell thickness t = Rout Rin , core
volume fraction f = (Rin /Rout )3 , permittivity of the inner
layer c , and permittivity of the outer layer s .
near fields has lead to new techniques, such as quanti-
tative measurements of the near-field heat flux between
the scanning thermal microscope tip and a planar sam-
ple at nanometer distances. An important aspect of this
topic is the fact that, for theoretical predictions, the tip
is usually modeled as sphere, however, in many of these
experiments a coated tip is used in measurement of near-
field thermal properties in probe-sample setups. It is
also shown that insufficiently cleaned probe (which acts
as a coating layer) or coverage material in such probe-
sample experiments leads to drastic change in the ther-
mal conductance23 . Accordingly, the synergistic effects
of coated particles should be considered and is important,
because it provides insight into the advantageous use of
CSNPs in thermal managements.
In this Letter, we investigate the radiative transfer
between core-shell nanoparticles. We show that using
CSNPs can drastically change the radiative heat trans-
fer compared with the radiative transfer between sin-
gle component nanoparticles, suggesting the presence of
new modes participating in the heat flux between such
nanoparticles. There are two types of CSNP investigated
in this research, i.e. SiO2 @Au and Au@SiO2 core-shell
nanoparticles. We demonstrate that the radiative heat
transfer in a dimer of Au@SiO2 (or SiO2 @Au) CSNPs not

only combine the optical signatures of silica and the plas-
monic properties of gold, but exhibits further enhanced
and expanded plasmonic tunability as well due to the di-
electric properties of the shell material surrounding the
core. The combination of these effects results in a giant
enhancement of the thermal conductance in a dimer of
silica-coated Au nanoparticles compared to that of bare
Au nanoparticles. On the other side, we show that the
reduction of several order of magnitude in the heat trans-
fer is possible between gold-coated silica nanoparticles
(SiO2 @Au CSNPs) than that of uncoated SiO2 nanopar-
ticles.
The schematic of the system under consideration is
sketched in Fig. (1). Two spherical CSNPs are located
at fixed distance of d from each other inside a trans-
parent dielectric of permittivity h . Nanoparticles are
kept at temperatures Ti (i = 1, 2), and exchanges en-
ergy via radiation. Each nanoparticle is characterized
by its core radius and shell thickness denoted by Rin ,
and t = Rout Rin respectively; where Rout is the ra-
dius the nanoparticle. Moreover, the core volume frac-
tion f = (Rin /Rout )3 = (1 + t/Rin )3 is introduced,
which represents the ratio of the core volume to the to-
tal volume of each CSNP. We assume that the size of
nanoparticles are small compared to the thermal wave-
length T = c~/kB T (wherein c is light velocity in the
vacuum, 2~ and kB are Planck and Boltzmann con-
stants, respectively). With this assumption and using the
Mies first coefficients24 , we approximated each CSNP by
fluctuating dipole with electric and magnetic polarizabil-
ities:
(s h )(c + 2s ) + f (c s )(h + 2s )
E = 3v
(s + 2h )(c + 2s ) + f (c s )(2s 2h )
v h ( ) + f 5/3 ( ) i
s h c s
H = (kh Rout )2 , (1b)
10 h
where
v = 43 Rout
3
is the volume of the CSNP, kh =
h /c, and c () and s () are the dielectric permit-
tivity of core and shell, respectively. To simplify our
analysis, we assume the radiative heat transfer in dimer
with identical CSNPs. To this end, CSNPs are as-
sumed to have same core (i.e., c 1,c = 2,c , Rin =
R1,in = R2,in ) and also same shell (i.e., s 1,s = 2,s ,
t = t1 = t2 ). Moreover, we take the dielectric function
h of the surrounding medium to be 1. The heat transfer
between two CSNP is modeled by the interaction of sim-
ple fluctuating dipoles. The associated net heat flux can
be described using the many-body radiative heat trans-
fer theory9,2527 , from which the mutual conductance at
small temperature mismatch (T1 T2 0) around tem-
perature T reads25
X Z d (, T )
G= T () , (2)
0 2 T gold is a core material and Lef f = 34 Rout
=E,H
~
where (, T ) = ~/[e KB T 1] is the mean energy of
a Plank harmonic oscillator in thermal equilibrium at
2
frequency and temperature T . The transmission coef-
ficient, T (), with contribution of electric ( = E) and
magnetic ( = H) dipole moments, denotes the energy
transmission probability between these nanoparticles at
frequency , and could be defined as5
" #
GG
T () = 2Im(1 )Im(2 )Tr ( = E, H). (3)
M M
Here = + G0 | |2 is the susceptibility of CSNP
with polarizability , and G0 = i(k 3 /6). Moreover,
for spherical particles we have M = [1 1 2 G2 ],
where 1 stands for identity operator, and the interac-
tion of nanoparticles in a dimer is accounted for by the
free space Green tensor G25 . The transmission proba-
bility in Eq. (3), is proportional to the imaginary parts
of the polarizability of nanoparticles, which can exhibit
a strong electric25 and/or magnetic28 dipole resonances.
The strengths and the frequencies at which these reso-
nances might occur depend on the material composition
of both the core and shell of nanoparticles as well as their
core volume fraction f . It is also straight forward to have
the condition for frequency with zero energy transmission
by requiring Eq. (3) to be zero, in which the effective po-
larizability of the CSNP equal to that of free space.
Let us now apply this theoretical framework to de-
scribe the thermal conductance in a dimer of CSNPs.
As we mentioned earlier, two types of CSNPs (SiO2 @Au
and Au@SiO2 ) are investigated in this research. We fo-
cus on the analysis of the thermal conductance at room
temperature (300 K). To determine if a resonance in the
transmission probability is realizable, where it occurs, its
strength, and its contribution to heat transfer; we need
,(1a) to know how the core/shell dielectric functions vary with
frequency. We have used the Drude-Lorentz model for
the dielectric function of SiO2 part of the effective polar-
izabilities of CSNPs29 . In order to make better link with
experiment, we have used Drude critical point model for
the dielectric function of bulk Au30 . More over, this di-
electric function is modified in order to take into account
the finite size effects in small core radius or small shell
thicknesses. We relay on the following radius-dependent
dielectric function for the metallic part of the CSNPs31
p2 p2
Au () = bulk () + , (4)
2 + ibulk 2 + i
where p = 8.9234 eV, bulk = 0.042389 eV, and vf =
1.4 106 m/s. Moreover = bulk + vf /Lef f is a radius-
corrected relaxation and vf is the Fermi velocity of con-
duction electrons. There are different approximate for-
mulas in the literature for effective mean free path of
electrons (Lef f ) which depend on the underlying model
of electron scattering from the metal boundaries32,33 . We
assume that Lef f = 34 Rin for Au@SiO2 CSNPs in which
R3 R3
2
in
2 in case of
out +Rin
SiO2 @Au CSNPs in which gold is a shell material.
We first investigate the thermal conductance in a dimer
of Au@SiO2 core-shell nanoparticles [see Figs. (2) and

Figure 2. (a) Normalized thermal conductance at T = 300 K
in a system composed of a dimer of 2 identical Au@SiO2 core-
shell nanoparticles with separation distance d = 120 nm for
fixed gold radius (Rin = 20 nm) as a function of the shell
(silica) thickness. The inset graph shows the contribution
of the electric and magnetic dipole moments to the thermal
conductance. (b) The transmission probability of the system
in part a.
(3)]. Here, we have taken two different cases to under-
stand the radiative heat transfer in this dimer. First,
we have considered Au@SiO2 CSNPs in which the in-
ner radius (Au core size) is fixed and the outer radii is
varying. The thermal conductance between two spherical
gold nanoparticles with radius R = 20 nm and separa-
tion distance d = 120 nm is shown in Fig. (2a) as a
function of the silica shell thickness (t = t1 = t2 ). The
result is normalized to the thermal conductance between
uncoated gold nanoparticles. It can be seen that cover-
ing Au nanoparticles with a SiO2 coating layer results in
a strong amplification in the heat transfer between gold
spheres. Moreover, when the silica coating layer has a
very large thickness, the thermal conductance saturates.
Some more insight on this amplification is given in the
inset of Fig. (2a) where the contribution of electric and
magnetic dipoles to the thermal conductance is repre-
sented. It is interesting to see that by increasing the SiO2
3
Figure 3. (a) Normalized thermal conductance at T = 300 K
in a system composed of a dimer of 2 identical Au@SiO2 core-
shell nanoparticles with separation distance d = 120 nm for
fixed outer radius (Rout = 20 nm) as a function of gold core
volume fraction. The inset graph shows the contribution of
the electric and magnetic dipole moments to the thermal con-
ductance. (b) The transmission probability of the system in
part a.
coating layer, the electric dipole contribution increases
whereas the magnetic contribution does not change sig-
nificantly. In addition to the dominant contribution of
electric dipole moments, a part of this enhancement is
due to increase in the size of CSNPs. As can be seen
in Fig. (2b), the main reason for the enhancement in
the thermal conductance is the increasing contribution
of SiO2 resonance modes in the transmission probabil-
ity between nanoparticles. As shown in this figure, the
surface resonance modes of gold core have slightly red-
shifted by silica coating. This is reasonable, due to an
increase in the local refractive index surrounding gold
nanoparticle produced by the SiO2 layer (in comparison
to the host material).
In the second case, we have discussed the thermal con-
ductance between two Au@SiO2 CSNPs with fixed outer
radius (Rout = 20 nm) as shown in Fig. (3a). The ther-
mal conductance is plotted as a function of gold core vol-

Figure 4. (a) Normalized thermal conductance at T = 300 K
in a system composed of a dimer of 2 identical SiO2 @Au core-
shell nanoparticles with separation distance d = 120 nm for
fixed silica radius (Rin = 20 nm) as a function of the shell
(gold) thickness. The inset graph shows the contribution of
the electric and magnetic dipole moments to the thermal con-
ductance. (b) The transmission probability of the system in
part a.
ume fraction and normalized to the thermal conductance
between two SiO2 bare nanoparticles. As we increase the
radius of the gold core, there is continuous reduction in
the thermal conductance. From the inset of Fig. (3a), it
is clear that the decrease in the electric conductance is
responsible for this reduction, even though the magnetic
contribution (with much less contribution) is an increas-
ing function of gold core volume fraction. One can see in
Fig. (3b) that peaks in the transmission probability (due
to the resonance of surface mode of silica nanoparticle)
slightly blue-shifted and decreased by increasing the gold
core volume fraction. Since the plasmon resonance fre-
quency of the gold core does not changes significantly by
size, the reduction in the thermal conductance can be at-
tributed to the decrease in the resonance surface modes
of SiO2 layer as it gets thinner.
Let us now examine what happens when a homoge-
neous polar core sphere is uniformly coated with a man-
4
Figure 5. (a) Normalized thermal conductance at T = 300 K
in a system composed of a dimer of 2 identical SiO2 @Au core-
shell nanoparticles with separation distance d = 120 nm for
fixed outer radius (Rout = 20 nm) as a function of silica core
volume fraction. The inset graph shows the contribution of
the electric and magnetic dipole moments to the thermal con-
ductance. (b) The transmission probability of the system in
part a.
tle of metallic composition. To this end, we investi-
gate the thermal conductance in a dimer of SiO2 @Au
CSNPs. The surface plasmons at both boundaries of
the gold layer interact with each other and bifurcate the
surface plasmon mode of a bare gold sphere into sym-
metric and asymmetric branches (known as the Frohlich
modes)24 . The symmetric type of the resonance exhibits
a plasmonic resonance at lower energies than the anti-
symmetric part. Due to this hybridization, the plasmon
resonance frequency of SiO2 @Au CSNPs could be pre-
cisely tuned by adjusting the thickness of the Au layer
or silica core volume15 , which allows one to control the
radiative heat transfer. Figure (4a) shows the influence
of the thicknesses of the gold layer on the thermal con-
ductance between two silica nanoparticles with radius
R = 20 nm and separation distance d = 120 nm. The
thermal conductance in a dimer is normalized to that of
uncoated SiO2 nanoparticles. Result indicates that coat-

ing a silica nanoparticle with a gold layer (t 0.5R)
leads to a decrease in the thermal conductance, while
with further increase of coating thickness the thermal
conductance increases. Despite the increasing contribu-
tion of magnetic dipole moments to thermal conductance,
the electric dipole moment has a dominant contribution
to the behavior of the thermal conductance as shown in
the inset of Fig. (4a). It is clear form Fig. (4b), that
presence of the gold coating layer, shields SiO2 core and
yields a strong reduction of SiO2 surface modes to the en-
ergy transmission probability. With SiO2 nanoparticles
inside, the SiO2 @Au CSNPs exhibit a well-known sym-
metric and anti-symmetric plasmonic resonances, which
broaden and displays a blue shift with thicker gold shell.
The increase in the contribution of symmetric mode in
the transmission probability is responsible for the in-
crease in the thermal conductance at larger shell thick-
nesses. The results are consistent with the reduction
in the intensity of dipolar resonance of the bare SiO2
nanoparticles16 , where the small variations in the thick-
ness of the gold shell have a less important influence on
the positions of the plasmon resonances but do influence
the general shape of the extinction curve17 .
We plot in Fig. (5a) the influence of the SiO2 core vol-
ume fraction on the thermal conductance between two
SiO2 @Au CSNPs with outer radius Rout = 20 nm sep-
arated by d = 120 nm apart. According to this figure,
increasing the core volume fraction leads to a significant
enhancement of thermal conductance. Compared to the
cases of SiO2 @Au with fixed core size discussed above,
the electric (magnetic) dipole contribution to thermal
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