Huicong Dong1, Bin Wen1, Yuwen Zhang2, Roderick Melnik3. 1. State Key Laboratory of Metastable Materials Science and Technology, Yanshan University, Qinhuangdao 066004, China. 2. Department of Mechanical and Aerospace Engineering, University of Missouri-Columbia, Columbia, Missouri 65211, United States. 3. The MS2Discovery Interdisciplinary Research Institute, Wilfrid Laurier University, 75 University Avenue West, Waterloo, Ontario N2L 3C5, Canada.
Abstract
To compare the thermal properties of heterogeneous and homogeneous interfaces, polycrystalline composites are proposed. Thermal properties of heterogeneous and homogeneous interfaces in the composites are investigated using molecular dynamics simulations. The results indicate that when the inflow of heat arises from the same material, phonon scattering at heterogeneous interfaces is stronger than that at homogeneous interfaces. The phonon wave packet simulations indicate that the stronger phonon scattering at heterogeneous interfaces is caused by the combined actions of transmission coefficients and transmission time.
To compare the thermal properties of heterogeneous and homogeneous interfaces, polycrystalline composites are proposed. Thermal properties of heterogeneous and homogeneous interfaces in the composites are investigated using molecular dynamics simulations. The results indicate that when the inflow of heat arises from the same material, phonon scattering at heterogeneous interfaces is stronger than that at homogeneous interfaces. The phonon wave packet simulations indicate that the stronger phonon scattering at heterogeneous interfaces is caused by the combined actions of transmission coefficients and transmission time.
Thermal conductivity
of polycrystalline materials is of great interest
because of its wide applications in many fields such as thermal barrier
coatings,[1] bioMEMs,[2] and micro-/nano-electromechanical devices.[3] It is well-known that a large number of grain boundaries exist in
polycrystalline materials,[4] thus leading
to a large increase in their thermal resistance when compared with
that of their corresponding single crystal.[5]The thermal resistance of polycrystalline materials can be
considered
as a series of connections between intragranular and intergranular
thermal resistances.[6] The intragranular
thermal resistance of polycrystalline materials is determined by the
thermal resistance and grain size of the bulk materials,[6] whereas the intergranular thermal resistance
is determined by the characters of the grain boundaries.[7] A previous study on the adjustment of polycrystalline
material thermal resistance was conducted mainly to change its grain
size; hence, it is natural to imagine that adjusting the grain boundaries’
characters may become another new way to adjust the thermal resistance
of polycrystalline materials. The grain boundary formed by different
phases, which is named heterogeneous interface, has been widely studied
in experiments[8−10] and in simulations.[11,12] Results indicate
that strong phonon scattering can be induced by heterogeneous interfaces.[8−12] Because of the asymmetry and lattice mismatch[13] of the heterogeneous interface, it probably induces stronger
phonon scattering compared with the grain boundary formed by the same
phase, which is named homogeneous interface.To verify this
hypothesis and study the effect of heterogeneous
and homogeneous interfaces on the thermal conductivity of polycrystalline
materials, polycrystalline composites are proposed, and the thermal
properties of heterogeneous and homogeneous interfaces are studied
in this work. Our simulated results demonstrate that when the inflow
of heat arises from the same material, phonon scattering at heterogeneous
interfaces is stronger than that at homogeneous interfaces because
of the combined actions of energy transmission coefficients and transmission
time.
Results and Discussion
To study the thermal properties
of heterogeneous and homogeneous
interfaces, diamond/SiCpolycrystalline composites have been proposed
as a prototype in this work. Figure S1 shows
a typical model of the diamond/SiCpolycrystalline composites with
periodic boundary conditions in three directions. As can be clearly
seen in Figure S1, the structure of the
polycrystalline composite is divided into three parts: the green parts
are the SiC phase, the blue parts are the diamond phase, and the others
are grain boundaries. The thermal conductivity of the composites with
a grain size of 2 nm is calculated using nonequilibrium molecular
dynamics (NEMD) simulations, and the results are plotted in Figure a. It can be seen
that our simulated thermal conductivity of polycrystallineSiC and
diamond agrees well with previously reported values,[6,14] indicating the reliability of NEMD simulation parameters used in
our work. As the SiC volume fraction increases, the thermal conductivity
of the composites decreases. Here, a Maxwell model,[15] which is the most popular model to describe the thermal
conductivity of composites with a spherical shape filler particle,
is also applied to express the thermal conductivity of diamond/SiCpolycrystalline composites. It has been demonstrated that the only
defect of the Maxwell model is that it disregards the thermal resistance
generated at the matrix and at the dispersed phase, and hence, it
always overestimates the thermal conductivity of the composites. Assuming
that polycrystalline diamond is the matrix phase and polycrystallineSiC is the dispersed phase, the thermal conductivity K of the diamond/SiCpolycrystalline composite can be obtained bywhere PSiC is
the volume fraction of polycrystallineSiC in composites and KDia and KSiC are
the thermal conductivities of polycrystalline diamond and SiC with
a grain size of 2 nm, respectively. By comparing the thermal conductivity
of diamond/SiCpolycrystalline composites using NEMD simulation with
the Maxwell model, it can be observed that the Maxwell model overestimates
the thermal conductivity of the polycrystalline composites. On the
basis of eq , the thermal
conductivity of the polycrystalline composites is calculated by combining
the thermal conductivities of polycrystalline diamond and SiC. According
to ref (6), the factors
that affect the thermal conductivity of polycrystalline materials
are grain boundaries (diamond/diamond interfaces for polycrystalline
diamond and SiC/SiC interfaces for polycrystallineSiC) and size effect.
Thus, in the calculation of the thermal conductivity of the composites
according to eq , although
the effect of homogeneous interfaces (diamond/diamond interfaces and
SiC/SiC interfaces) and the size effect on polycrystalline composites
have been considered, the thermal resistance generated at the matrix
(polycrystalline diamond) and at the dispersed phase (polycrystallineSiC) has been disregarded. Therefore, it can be deduced that the overestimation
of thermal conductivity by the Maxwell model for diamond/SiCpolycrystalline
composites may be caused by the larger thermal resistance of the heterogeneous
interface than that of the homogeneous interface.
Figure 1
Thermal transmission
properties in diamond/SiC polycrystalline
composites. (a) Variation of thermal conductivity for diamond/SiC
polycrystalline composites; the grain size is 2 nm, and the SiC volume
fraction ranges from 0 to 100%. [a] refers to ref (5) and [b] refers to ref (13). (b) Thermal resistances
for (001) heterogeneous and homogeneous interfaces with different
twist angles. RDia→SiC and RSiC→Dia are the thermal resistances of
diamond/SiC heterogeneous interfaces when the heat flux transmits
from diamond to SiC and in the opposite direction, respectively. RDia→Dia and RSiC→SiC are the thermal resistances for diamond/diamond and SiC/SiC homogeneous
interfaces, respectively.
Thermal transmission
properties in diamond/SiCpolycrystalline
composites. (a) Variation of thermal conductivity for diamond/SiCpolycrystalline composites; the grain size is 2 nm, and the SiC volume
fraction ranges from 0 to 100%. [a] refers to ref (5) and [b] refers to ref (13). (b) Thermal resistances
for (001) heterogeneous and homogeneous interfaces with different
twist angles. RDia→SiC and RSiC→Dia are the thermal resistances of
diamond/SiC heterogeneous interfaces when the heat flux transmits
from diamond to SiC and in the opposite direction, respectively. RDia→Dia and RSiC→SiC are the thermal resistances for diamond/diamond and SiC/SiC homogeneous
interfaces, respectively.To verify the deduction and study the different effects of
heterogeneous
and homogeneous interfaces on the thermal conductivity of diamond/SiCpolycrystalline composites, thermal resistances of (001) heterogeneous
(diamond/SiC) and homogeneous (diamond/diamond, SiC/SiC) interfaces
with different twist angles were simulated. The lengths of the simulation
cells used for the thermal resistance calculation are all 40 nm, and
the effect of heat direction on the heterogeneous interface thermal
resistance is taken into account. The calculated results are summarized
in Figure b, and it
can be seen that the thermal resistance of heterogeneous and homogeneous
interfaces varies with different twist angles. The mean values of
heterogeneous interface thermal resistance when heat flux transmits
from diamond to SiC, RDia→SiC,
and in the opposite direction, RSiC→Dia, are 3.85 × 10–10 and 7.63 × 10–10 m2 K/W, respectively. For homogeneous
interfaces, the mean values of thermal resistance for diamond/diamond
interfaces, RDia→Dia, and SiC/SiC
interfaces, RSiC→SiC, are approximately
1.92 × 10–10 and 4.69 × 10–10 m2 K/W, respectively; these values are consistent with
the previous simulated results.[6,14] By comparing the thermal
resistances of heterogeneous and homogeneous interfaces, it can be
found that the mean value of RDia→SiC is larger than that of RDia→Dia, and RSiC→Dia is larger than RSiC→SiC. Thus, it can be concluded that
when the inflow of heat arises from the same material, phonon scattering
at heterogeneous interfaces is stronger than that at homogeneous interfaces,
confirming our deduction above. The strong phonon scattering at the
heterogeneous interfaces has also been verified in many other systems
experimentally.[8−10] Moreover, it can also be observed in Figure b that RSiC→Dia is larger than RDia→SiC, indicating the thermal rectification at heterogeneous interfaces,
which has also been observed in other systems.[16,17] It has been reported that the rectification is caused by different
thermal conductivities of materials on the two sides of the heterogeneous
interface.[17]By combining the calculated D-values between the
heterogeneous and homogeneous interface thermal resistances and the
Maxwell model, the thermal conductivity of diamond/SiC composites
has been recalculated in a modified model, which is expressed by the
following expressionwhere KMaxwell is the thermal conductivity
of the composites in the Maxwell model,
ΔRK is the D-value
between the heterogeneous and homogeneous interface thermal resistances
when the inflow of heat arises from the same material, d is the grain size, and P is the heterogeneous interface
fraction that is calculated based on the probability theory, and it
is a parameter related to the SiC volume fraction.It is well-known
that three kinds of interfaces in diamond/SiCpolycrystalline composites exist, namely, diamond/diamond, SiC/SiC,
and diamond/SiC interfaces. According to the probability theory, the
fraction of diamond/diamond interfaces is (1 – PSiC)2, the fraction of SiC/SiC interfaces is PSiC2, and the fraction of diamond/SiC
interfaces is 2PSiC(1 – PSiC). Considering the rectification of heterogeneous
interfaces, diamond/SiC interfaces are divided into two kinds: One
kind is the interface when the inflow of heat arises from diamond,
assuming that the fraction of this kind of interface in the total
heterogeneous interfaces equals the fraction of diamond/diamond interfaces
in the total homogeneous interfaces(1 – PSiC)2/[PSiC2 + (1 – PSiC)2]; thus,
the final fraction of this kind of interface in the total interfaces
is 2PSiC(1 – PSiC)3/[PSiC2 + (1 – PSiC)2]. The other kind is the interface when the inflow of heat arises
from SiC; in the same way, the final fraction of this kind of interface
in the total interfaces can be obtained as 2PSiC3(1 – PSiC)/[PSiC2 + (1 – PSiC)2]. As a result, eq leads toThe calculated results based on eq have been plotted in Figure a; it can be seen that our modified model
coincides with the NEMD simulation results, well-indicating that the
stronger phonon scattering at the heterogeneous interfaces than that
at the homogeneous interfaces is indeed the reason for the overestimation
of the Maxwell model.Although the above-calculated interface
thermal resistances can
reflect the stronger phonon scattering at heterogeneous interfaces,
they are obtained by averaging the phonon scattering properties over
the entire phonon frequencies. To understand the frequency-dependent
phonon scattering at interfaces by considering contributions from
phonons at different frequencies and in different branches, the interface
thermal resistance R is expressed as[18]where is the
wave vector, λ is the phonon branch, ℏ is the Planck constant, ω(,
λ) is the phonon frequency with the wave vector in branch λ, n(ω, T) is the Bose occupation factor at temperature T, α(, λ) is
the energy transmission coefficient across the interface, and v(, λ) is the phonon
group velocity across the interface. Thus, it can be concluded that
when the inflow of heat arises from the same material, the factors
that lead to the difference between the heterogeneous and homogeneous
interface thermal resistances are the transmission coefficient and
the phonon group velocity across the interfaces.To obtain the
transmission coefficient and the group velocity across
the interface, phonon wave packet (PWP) method[19,20] is used. In this paper, PWP simulations on phonon scattering at
diamond/SiC (twist angle is 0°), diamond/diamond (twist angle
is 53.13°), and SiC/SiC interfaces (twist angle is 53.13°)
are carried out as examples. Figure a shows the snapshots of a wave packet arising from
diamond scattering at diamond/SiC and diamond/diamond interfaces at
different times with two instanced frequencies (1.32 and 12.92 THz).
It can be seen that for the wave packet with 1.32 THz, only 4% of
the incident energy is reflected at the heterogeneous interface, and
nearly all incident energy can transmit across the homogeneous interface.
For the wave packet with 12.92 THz, approximately 20% of the energy
is reflected at the heterogeneous interface, and a significant portion
of the incident energy is scattered into modes different from the
incident wave packet. Approximately 10% of the energy is reflected
at the homogeneous interface, and the modes of scattered energy are
the same as those of the incident energy.
Figure 2
PWP simulations on heterogeneous
and homogeneous interfaces. (a)
Snapshots of the Z displacement of atoms for the
wave packet with frequencies of 1.32 and 12.92 THz. The wave packet
arises from diamond, and it scatters at (001) diamond/SiC (twist angle
is 0°) and diamond/diamond (twist angle is 53.13°) interfaces
separately. The vertical black line at Z = 3556 Å
indicates the location of the interface. (b) Frequency-dependent energy
transmission coefficients for heterogeneous and homogeneous interfaces.
αDia→SiC and αSiC→Dia are the transmission coefficients for (001) diamond/SiC interfaces
(twist angle is 0°) when the wave packet transmits from diamond
to SiC and in the opposite direction, respectively. αDia→Dia and αSiC→SiC are the transmission coefficients
for (001) diamond/diamond and SiC/SiC interfaces (twist angle is 53.13°),
respectively. Inset: Comparison of LA phonon dispersion curves between
diamond and SiC single crystals.
PWP simulations on heterogeneous
and homogeneous interfaces. (a)
Snapshots of the Z displacement of atoms for the
wave packet with frequencies of 1.32 and 12.92 THz. The wave packet
arises from diamond, and it scatters at (001) diamond/SiC (twist angle
is 0°) and diamond/diamond (twist angle is 53.13°) interfaces
separately. The vertical black line at Z = 3556 Å
indicates the location of the interface. (b) Frequency-dependent energy
transmission coefficients for heterogeneous and homogeneous interfaces.
αDia→SiC and αSiC→Dia are the transmission coefficients for (001) diamond/SiC interfaces
(twist angle is 0°) when the wave packet transmits from diamond
to SiC and in the opposite direction, respectively. αDia→Dia and αSiC→SiC are the transmission coefficients
for (001) diamond/diamond and SiC/SiC interfaces (twist angle is 53.13°),
respectively. Inset: Comparison of LA phonon dispersion curves between
diamond and SiC single crystals.Figure b
shows
the frequency-dependent transmission coefficients α for wave
packets comprising longitudinal acoustic (LA) phonons scattering at
heterogeneous and homogeneous interfaces. It can be seen that the
transmission coefficients depend strongly, but not smoothly, on the
frequency of the incident wave, ω. For the wave packet arising
from diamond, the transmission coefficient at the diamond/SiC interface,
αDia→SiC, is kept at approximately 0.96 when
ω < 6 THz. Then, it decreases from 0.95 to approximately
0.5 monotonically for 6 THz < ω < 18.3 THz, and it sharply
drops to zero at a frequency of 19.53 THz. Moreover, αDia→SiC remains at zero for frequency ranging from 19.53 to 34.11 THz because
there are no available LA modes with frequencies larger than 18.3
THz in SiC (see the inset in Figure b). For the diamond/diamond interface, the transmission
coefficient αDia→Dia is close to 1 when ω
< 6 THz. Then, it decreases from 0.97 to approximately 0.75 monotonically
when 6 THz < ω < 16.9 THz, and αDia→Dia decreases from 0.99 to 0.235 in a fluctuation way for 16.9 THz <
ω < 34.11 THz. Comparison between αDia→SiC and αDia→Dia shows that, with phonon frequency
ranging from 1.32 to 34.11 THz, αDia→SiC is
lower than αDia→Dia all through the considered
range, making a contribution to stronger phonon scattering at diamond/SiC
heterogeneous interfaces than that at diamond/diamond homogeneous
interfaces. For the wave packet arising from SiC, both transmission
coefficients at diamond/SiC heterogeneous and SiC/SiC homogeneous
interfaces, αSiC→Dia and αSiC→SiC, almost remain unchanged for ω < 5 THz. After that, a monotonic
variation of transmission coefficients occurs for 5 THz < ω
< 9 THz, and finally they both fluctuate for 9 THz < ω
< 18.3 THz. Although the variation tendencies of αSiC→Dia and αSiC→SiC are similar, the values of
αSiC→Dia and αSiC→SiC are different from each other when the frequency of the incident
wave packet is the same. Note also that the value of αSiC→Dia is smaller than αSiC→SiC for ω <
9 THz, whereas αSiC→Dia is larger than αSiC→SiC for ω > 9 THz. Moreover, it can also
be
observed in similar cases throughout that at a low frequency (ω
< 6 THz for the wave packet arising from diamond and ω <
5 THz for the wave packet arising from SiC), transmission coefficients
at both heterogeneous and homogeneous interfaces are high, and they
are very close to a constant, which can also be observed in other
systems.[18,21] When the incident frequency is low, the
phonons have a long wavelength, and they behave like classical plane
waves.[22] Under this condition, the acoustic
mismatch (AM) model[22] is valid, and the
transmission coefficients αAB between material A
and material B can be obtained bywhere Z = ρv is the acoustic impedance, ρ is the mass density,
and v is the phonon group velocity. When the incident
phonon frequency is low, the phonon group velocities on both sides
of the homogeneous interfaces are extremely large. Despite the effect
of atomic plane orientation, the group velocities at both sides of
homogeneous interfaces are very close to each other. As a result,
according to the AM model, the transmission coefficients calculated
for homogeneous interfaces are very close to 1.[20] For the heterogeneous interface, the calculated transmission
coefficient in the AM model is approximately 0.96 based on the acoustic
impedance difference between diamond and SiC.[23,24] The estimation of transmission coefficients for the heterogeneous
and homogeneous interfaces in eq matches well with the PWP simulation results. For the wave
packet with high frequency (ω > 6 THz for the wave packet
arising
from diamond and ω > 5 THz for the wave packet arising from
SiC), a monotonically decreased tendency of transmission coefficients
first occurs with increased frequencies, which results from the decreasing
phonon wavelength. After that, the transmission coefficients fluctuate
with increased frequency, and this phenomenon has been demonstrated
to be closely related to the mismatch of phonon density of states
between the grain and interface regions.[25]Besides the energy transmission coefficient, the phonon group
velocity
across the interface is another factor that causes differences between
the heterogeneous and homogeneous interface thermal resistances according
to eq , and it can be
reflected by the wave packet velocity across the interface. In the
PWP simulation, the widths of wave packets arising from the same material
across heterogeneous and homogeneous interfaces are the same (refer
to Discussion 1). Thus, for wave packets
with the same origin, comparison of velocities between the wave packets
across heterogeneous and homogeneous interfaces can be estimated by
comparing the transmission times Γ. The transmission time is
the time difference between the start and the end times of wave packet
energy transmission between the two sides of the interface. Figure a shows the start
and end times for a wave packet with an instanced incident frequency
1.15 THz arising from diamond across diamond/SiC and diamond/diamond
interfaces. It can be seen that when the wave packet goes across the
diamond/SiC interface, energy transmission starts at 1.85 ps and finishes
at 10.4 ps. When the wave packet goes across the diamond/diamond interface,
the start and end times are 2.25 and 9.5 ps, respectively. Different
start and end times for wave packet across heterogeneous and homogeneous
interfaces can also be observed in some other situations, as shown
in Figure S2. By calculating the time difference
between the start and end times of the wave packet energy transmission,
the transmission times for the wave packet across heterogeneous and
homogeneous interfaces at different frequencies can be obtained. As
can be seen in Figure b, for the wave packet arising from diamond, when the incident frequency
ranges from 1.15 to 18.3 THz, the transmission time for wave packet
across the diamond/SiC interface, ΓDia→SiC, varies between 6.15 and 7.3 ps, whereas the transmission time for
the diamond/diamond interface, ΓDia→Dia, varies
between 7.2 and 11 ps. Comparison between ΓDia→SiC and ΓDia→Dia indicates that when the incident
frequency is the same, the value of ΓDia→SiC is larger than ΓDia→Dia. Similarly, for
the wave packet arising from SiC, it can also be observed that the
transmission time for the wave packet across the diamond/SiC interface,
ΓSiC→Dia, is larger than that across the SiC/SiC
interface, ΓSiC→SiC. Thus, it can be concluded
that for the wave packet with the same origin, heterogeneous interfaces
prolong the energy transmission time compared with the homogeneous
interfaces. This is another important reason for stronger phonon scattering
at heterogeneous interfaces than that at homogeneous interfaces.
Figure 3
Comparison
of transmission times for the wave packet across heterogeneous
and homogeneous interfaces. (a) Start and end times of energy transmission
for the wave packet arising from diamond with 1.15 THz across diamond/SiC
and diamond/diamond interfaces. σDia→SiC and
σDia→Dia are the transmission rates for the
wave packet across diamond/SiC and diamond/diamond interfaces, respectively.
Inset: Magnified start and end times of energy transmission for diamond/diamond
and diamond/SiC interfaces. (b) Transmission times for the wave packet
across heterogeneous and homogeneous interfaces. ΓDia→SiC and ΓDia→Dia are the transmission times
for the wave packet arising from diamond across diamond/SiC and diamond/diamond
interfaces, respectively. ΓSiC→Dia and ΓSiC→SiC are the transmission times for the wave packet
arising from SiC across diamond/SiC and SiC/SiC interfaces, respectively.
Comparison
of transmission times for the wave packet across heterogeneous
and homogeneous interfaces. (a) Start and end times of energy transmission
for the wave packet arising from diamond with 1.15 THz across diamond/SiC
and diamond/diamond interfaces. σDia→SiC and
σDia→Dia are the transmission rates for the
wave packet across diamond/SiC and diamond/diamond interfaces, respectively.
Inset: Magnified start and end times of energy transmission for diamond/diamond
and diamond/SiC interfaces. (b) Transmission times for the wave packet
across heterogeneous and homogeneous interfaces. ΓDia→SiC and ΓDia→Dia are the transmission times
for the wave packet arising from diamond across diamond/SiC and diamond/diamond
interfaces, respectively. ΓSiC→Dia and ΓSiC→SiC are the transmission times for the wave packet
arising from SiC across diamond/SiC and SiC/SiC interfaces, respectively.Moreover, by applying the inverse
relationship between the wave
packet velocity and the transmission time (v ∝
1/Γ) in eq , when
the wave packet arises from the same material, for a certain incident
frequency, the ratio between the thermal resistances of heterogeneous
(RHeter) and homogeneous (RHomo) interfaces can be obtained bywhere αHomo and ΓHomo are the transmission coefficient and the transmission
time for the homogeneous interface and αHeter and
ΓHeter are the transmission coefficient and the transmission
time for the heterogeneous interface. Thus, the frequency-dependent RHeter/RHomo can
be obtained by applying the transmission coefficient and transmission
time in PWP simulations. As shown in Figure , for the wave packet arising from diamond,
when the incident frequency ranges from 1.15 to 18.3 THz, the value
of RDia→SiC/RDia→Dia varies between 1.2 and 2.6, and this range includes
the ratio between RDia→SiC and RDia→Dia in NEMD simulations. For the
wave packet arising from SiC, when the incident frequency ranges from
1.15 to 16.9 THz, RSiC→Dia/RSiC→SiC varies between 0.17 and 1.52,
also including the value of RSiC→Dia/RSiC→SiC in NEMD simulations.
Thus, it can be concluded that when heat flow arises from the same
material, stronger phonon scattering at heterogeneous interfaces than
that at homogeneous interfaces is caused by the combined actions of
transmission coefficients and transmission time.
Figure 4
Frequency-dependent ratios
between heterogeneous and homogeneous
interface thermal resistances. RDia→SiC/RDia→Dia is the ratio between
diamond/SiC and diamond/diamond interface thermal resistances when
the inflow of heat arises from diamond, and RSiC→Dia/RSiC→SiC is
the ratio between diamond/SiC and SiC/SiC interface thermal resistances
when the inflow of heat arises from SiC.
Frequency-dependent ratios
between heterogeneous and homogeneous
interface thermal resistances. RDia→SiC/RDia→Dia is the ratio between
diamond/SiC and diamond/diamond interface thermal resistances when
the inflow of heat arises from diamond, and RSiC→Dia/RSiC→SiC is
the ratio between diamond/SiC and SiC/SiC interface thermal resistances
when the inflow of heat arises from SiC.
Conclusions
In summary, diamond/SiCpolycrystalline composites
are proposed
as a prototype for studying the thermal properties of heterogeneous
and homogeneous interfaces. The thermal resistances of heterogeneous
and homogeneous interfaces are obtained using NEMD simulations. The
results indicate that when the inflow of heat arises from the same
material, phonon scattering at heterogeneous interfaces is stronger
than that at homogeneous interfaces. PWP simulations are carried out
to analyze the different scattering mechanisms at the heterogeneous
and homogeneous interfaces, and the results show that the stronger
phonon scattering at heterogeneous interfaces is caused by the combined
actions of energy transmission coefficients
and transmission time. Our findings provide a practical guidance on
how to adjust the thermal resistance of polycrystalline materials
by introducing heterogeneous interfaces in polycrystalline materials.
Simulation
Section
Thermal Conductivity Calculation of Diamond/SiC Polycrystalline
Composites
The atomic structures of diamond/SiCpolycrystalline
composites are built with in-house software using the three-dimensional
Voronoi tessellation method[26] (details
can be found in Discussion 2). The grain
sizes of composites are 2 nm, and the total number of composite grains
in the simulation is 16. The diamond and SiC grains are distributed
randomly in the composites, and the SiC volume fraction ranges from
0 to 100%, which is controlled by varying the number of diamond grains
and SiC grains. To calculate the thermal conductivity of diamond/SiCpolycrystalline composites, nonequilibrium molecular dynamics simulations
are carried out (details can be found in Discussion 3). All simulations are conducted in the LAMMPS[27] package at a temperature of 300 K. Tersoff potential,[28] which has been verified accurate for thermal
conductivity calculations, is used to describe C–C and Si–C
bonding interactions. After energy minimization, the simulation structures
are first equilibrated for 40 ps under the NPT ensemble with a constant
pressure of 1 bar. After they are fully equilibrated, NEMD simulations
are carried out on the relaxed structures to establish temperature
gradients. Finally, thermal conductivity is calculated based on Fourier’s
law.[6]
Interface Thermal Resistance
Calculation
To calculate
the interface thermal resistance, structures of heterogeneous and
homogeneous interfaces with different twist angles are created (refer
to Discussion 4). To avoid the effect of
sample length on the interface thermal resistance, the length of the
simulation cells are chosen as 40 nm. NEMD simulations[29,30] are performed to calculate the interface thermal resistance with
a time step of 1 fs, and the temperature used is 300 K in all simulations.
Tersoff potential[28] is used to describe
C–C and Si–C bonding interactions. Periodic boundary
conditions are applied in all three directions. Structural relaxation
and temperature equilibration are first carried out with the NPT ensemble.
Then, heat flux is imposed on the relaxed structures with the NVE
ensemble, as shown in Figure S5a; a temperature
discontinuity (ΔT) appears at the interface,
as shown in Figure S5b. The interface thermal
resistance R is calculated as the ratio between ΔT and the heat flux density J passing through
the interface[14]
Energy
Transmission Coefficients Calculation
To calculate
the energy transmission coefficients, the PWP method (refer to Discussion 1) is used by implementing it in the
LAMMPS package.[31] The PWPs are formed from
the linear combinations of vibrational eigenstates, which are found
by diagonalizing the dynamical matrix of the perfect crystal.[19] Following Schelling et al.,[19] Gaussian wave packets propagating from the left of the
interface to the right are applied along the [001] direction. In PWP
simulations, all wave packets are LA waves, and the length of our
simulated system is 2000a (2000a diamond or SiC for homogeneous interfaces
and 1000a diamond and 1000a SiC for heterogeneous interfaces) in the
propagation direction. Periodic boundary conditions are applied in
all three directions. Tersoff potential[28] is used to describe C–C and C–Si bonding interactions.
The ambient temperature is 0 K,[20] the ensemble
used is NVE, and time step is chosen as 1 fs. The energy transmission
coefficient α can then be computed aswhere ER is the
transmitted energy on the right side of the interface and E0 is the energy of the initial wave packet at
time t = 0 ps.
Energy Transmission Time
Calculation
To calculate the
energy transmission time, the time-dependent energy transmission coefficient
is calculated first, as shown in Figure S6. Then, the time-dependent transmission coefficient is differentiated
with respect to time, and the energy transmission rate σ at
different moments is obtained, as shown in Figure a. It can be seen that the transmission rate
fluctuates between −1 and 1. The first moment at which the
absolute value of transmission rate equals 0.01 is defined as the
start time of energy transmission, and the final moment at which the
absolute value of transmission rate equals 0.01 is defined as the
end time of energy transmission. Energy transmission time Γ
can then be obtained by calculating the time difference between the
start ΓS and end time ΓE of energy
transmission