Journal of Crystal Growth 542 (2020) 125687

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Journal of Crystal Growth

journal homepage: www.elsevier.com/locate/jcrysgro

A thermodynamically-consistent multi-physics framework for crystallization T

of phase-change material
⁎
Hamed Attariania, , Weisong Wangb, Rafał Gałekc
a
Department of Mechanical and Materials Engineering, Wright State University, Dayton, OH 45431, USA
b
Department of Electrical Engineering, Wright State University, Dayton, OH 45431, USA
c
Department of Thermodynamics, Faculty of Mechanical Engineering and Aeronautics, Rzeszów University of Technology, 35-959 Rzeszów, Poland

A R T I C LE I N FO A B S T R A C T

Communicated by Chung wen Lan Phase Change Materials (PCMs) have a diverse set of technological applications, including phase-change random
Keywords: access memory devices (PCRAMs), and their behavior can be understood based on a complex set of coupled
A1. Computer simulation physical phenomena, e.g., heat transfer, phase transition, and thermoelectric effects. A detailed understanding of
A1. Nucleation these phenomena and their interactions during the operation of a cell results in an efficient and compact design
A1. Growth models of the devices. This paper reports our development of a coupled, thermodynamically-consistent model to study
A1. Heat transfer the interplay among various parameters in PCRAMs, e.g., temperature, electrical current, thermoelectric effect,
B1. Nanomaterials and crystal nucleation/growth. A Phase-Field (PF) model was developed to model the phase transition (PT).
B2. Dielectric materials
Also, we show that incorporating the heat of crystallization in heat transfer model results in identifying a self-
heating mechanism in PCRAMs and consequently self-sustaining crystallization; crystallization continues even
after the external voltage is turned off.

1. Introduction
Within the many types of multi-functional materials, phase change
materials (PCMs) are among the first promising materials that have
been discovered and researched [1,2]. PCMs have significant contrasts
in their physical properties, e.g., optical, and electrical properties, due
to their phase transitions (PTs). For example, pristine vanadium dioxide
(VO2), as a metal oxide transition (MOT) material, changes from being
a dielectric to being conductive when the temperature rises above
68 °C. This reversible PT that is accompanied with a large contrast in
physical properties has resulted in a wide variety of technological ap-
plications for PCMs, e.g., smart windows, microbolometers, and elec-
tronic devices. Specifically, incorporating PCM in electronics devices,
e.g., phase-change random access memory device (PCRAM), could
provide further improvements in modern electronic systems, such as
enhanced performance, reduced size, lowered cost, and less complexity.
In this paper, we focus on a less researched, but potentially more
promising, chalcogenide phase change material, i.e., germanium-anti-
mony-tellurium (GeSbTe or GST). Unlike vanadium oxide, GST is a non-
volatile, phase-change material that could be highly beneficial in var-
ious applications, such as memory and neuromorphic computing with
devices that have much simpler structures and less power consumption
than traditional, transistor-based storage elements. As-deposited GST is
amorphous and has high resistivity. However, its electrical resistivity
decreases dramatically at about 150 °C due to the crystallization of the
material. The decrease in the resistivity could be as much as four orders
of magnitude [3], and this decrease is not reversed unless the melting is
followed by a quenching process to trigger amorphization of the crystal.
Any large variation in electrical resistivity due to PT is resulted in in-
formation loss in PCRAMs; note that the working principle of PCRAMs
is based on large electrical resistivity contrast between amorphous
(high electrical resistivity) and crystalline phase (low electrical re-
sistivity). Considering all of the merits that GST could offer to futuristic
electronic systems, the theoretical study of PCMs serves as a central
piece to further understand/design novel materials for electronic ap-
plications.
There have been numerous studies on the crystallization of amor-
phous GST (a-GST), but those models ignored the coupling among the
variables [4] or implemented phenomenological equations for crystal-
lization [5–7] rather than using thermodynamically-consistent models.
The only phase field (PF) model for GST focused simply on iso-thermal
annealing [8]. The developers used a fitting parameter to control the
nucleus growth velocity, and the nucleation rate and growth velocity
were valid only in a limited temperature range. Their model was used
successfully to investigate data retention in a-GST at specific tempera-
tures. Therefore, a generic, thermodynamically-consistent model for

⁎
Corresponding author.
E-mail address: hamed.attariani@wright.edu (H. Attariani).

https://doi.org/10.1016/j.jcrysgro.2020.125687
Received 21 January 2020; Received in revised form 17 April 2020; Accepted 20 April 2020
Available online 21 April 2020
0022-0248/ © 2020 Elsevier B.V. All rights reserved.
H. Attariani, et al. Journal of Crystal Growth 542 (2020) 125687

Fig. 1. The applied voltage keeps the temperature between the glass transition temperature, Tg, and the melting temperature, Tm, i.e., the set process; b) Schematic
of the device: The as-deposited a-GST is confined between two electrodes; c) Boundary condition for the 25 nm a-GST.

Fig. 2. Simulation flowchart. The crystal growth velocity is required to calculate mobility in PF model. Note that VG is a function of temperature.

predicting the response of the PCMs to various external stimuli is still a
necessity. Here, we developed a high-fidelity PF model to cover the
interaction among various phenomena over a wide range of tempera-
tures. In addition, to increase the accuracy of the model, more accurate
representations of growth velocity and nucleation rate were used based
on ultra-fast measurement techniques [9]. These results can be used to
design PCRAM devices that are more efficient.
2. Computational Model
The main objective of this study is to use a coupled multi-physics
model to acquire a better understanding of the underlying physics of
the crystallization of as-deposited a-GST. In the set process, one needs
to keep the temperature between the glass transition temperature (Tg)
and the melting temperature (Tm) to transform the a-GST to crystalline
GST (c-GST) (Fig. 1a). Fig. 1b-c show the schematic of our device, a
confined a-GST with a thickness of 25 nm, and corresponding boundary

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H. Attariani, et al. Journal of Crystal Growth 542 (2020) 125687

Table 1 Neumann BC is implemented for the order parameter on the top/

Material constants. bottom boundaries. The Multi-physics, Object-Oriented, Simulation
κ (ev/nm) [8] 0.165 S(mV/K)[15] 0.35 Environment (MOOSE) [10] was used to model the coupled physics
Hf (ev/nm3) [8] 2.616 γ (ev/nm2) [16] 0.5 mathematical framework, i.e., PF, nucleation/growth, heat conduction,
ΔHa, c (ev/nm3) [7] 1.32 Tg (K) [9] 472 thermoelectric effect, and electrical current. Also, the mesh adaptive
ratom (nm) [9] 0.1365 Tm (K) [16] 889 algorithm was used to increase the computational efficiency and also to
λ (nm) [9] 0.299 cp,a, cp,c (J/kgK) [7] 440, 202
resolve the interface between the crystal and amorphous phases. The
Rhyd (nm) [9] 0.1365 m [9] 140
μ (Pa.s) [9] 0.012 ρa, c (kg/m3) [17] 6150 details of the multi-physics equations that were developed are sum-
Ka, Kc (W/mK) [18] 0.19, 0.57 Vm(nm3) [4] 0.29 marized in the following sections.

conditions (BCs). A 245-µm TiN electrode was replaced by its corre-
sponding thermal resistivity, i.e., RT = l/ k , to consider the heat transfer
via the top/bottom boundaries, Fig. 1c. Here, l is the length of electrode
and k is thermal conductivity. The periodic boundary condition (PBC) is
used for order parameter and temperature, T, on the lateral sides to
mimic a thin film that has a large width. Also, the gradient of electrical
current, ∇ . J , is set to zero for the right/left boundaries. Then, the
2.1. Crystallization model
The Allen–Cahn formalism, Eq.1, was implemented to model the
temporal evolution of crystallization in the set process. The order
parameter, η, was used to represent various phases (structural order
parameter); η = 0 shows the amorphous phase, and η = 1 indicates the
crystalline phase.

Fig. 3. Crystallization for iso-thermal annealing at T = 463 K and 488 K: a) Evolution of the crystal volume fraction based on the PF and the JMAK model for
T = 488 K; b-d) nucleation and growth at t = 18, 22, and 30 s. The structural order parameter is varying varied between 0 and 1, and it is shown by the eta symbol on
the corresponding color legend.

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H. Attariani, et al. Journal of Crystal Growth 542 (2020) 125687

Fig. 4. The progress of crystallization and the temperature distribution in the Set process with constant voltage: a-f) phase and temperature distribution at t = 45.1,
55.6, 62.1, 69.1, 70.1, and 72.7 ns. The structural order parameter varied between 0 and 1, and it is shown by the eta symbol on the corresponding color legend.

∂η dF barrier-less melting/quenching, i.e., the reset process in PCRAMs.

= −Lη [ − κ∇2 η ]
∂t dη (1)

where F, Lη, and κ are Helmholtz free energy, kinetic coefficients, and 2.2. Heat transfer model
gradient energy coefficient, respectively. The kinetic coefficient is a
function of growth velocity (VG), L η = VG r ∗/ κ , where r ∗ represents the The voltage applied via the electrodes causes Joule heating to occur
radius of the critical nucleus, i.e., r ∗ = 2γ /ΔG, where γ is the surface and raises the device temperature. A coupled heat conduction equation
energy, and ΔG = Hf 1 − ( T
Tm ). The Helmholtz free energy per unit [7], Eq. (3), was used to model the evolution of the temperature in a-
GST.
volume is:

T⎞ 2 T⎞ 2 dT
F(η , T) = 3Hf ⎛1 −⎜ η (1 − η)2 − Hf ⎛1 −
⎟ ⎜ η (3 − 2η)
⎟ ρCp − ∇∙ (k∇T ) = −∇V ∙J − ∇∙ (JST ) + QH
Tm ⎠ Tm ⎠ (2) dt (3)
⎝ ⎝
where Hf, T, and Tm are latent heat, temperature, and the melting where ρ is density, Cp is heat capacity, k is thermal conductivity, ΔHa, c
temperature of GST, respectively. The first term defines a temperature is the latent heat of crystallization, S is the Seebeck coefficient, and
dη
dependent double-well barrier between phases, and the second term is QH = dt × ΔHa, c (T ) . The first two terms on the right side of Eq. (3)
thermal energy. In this model, the height of double-well barrier energy represent the Joule heating and thermoelectric phenomenon. The
reduces with an increase in temperature which represents a more rea- Poisson equation (electrical model) should be solved to determine the
listic scenario and reduce the number of calibration parameters. This electrical current, J, across the thickness of the GST and then entered in
consistent thermodynamic potential also can be used to model the Eq. (3). (See section 2.3.)

4
H. Attariani, et al.
Fig. 5. Steady state nucleation rate and growth velocity below the GST melting
temperature.
2.3. Electrical Model
In the current model, a constant voltage, i.e., 0.5 V, was applied to
the GST film to induce a thermal gradient across the layer. The coupled
Poisson’s equation was used [11] to simulate the electrical current
across the a-GST and also the thermoelectric current.
∇∙J = ∇∙ (−σ ∇V − σS∇T ) = 0 (4)
where J is the electric current, σ is electrical conductivity, and V is
the electric potential. Variation of electrical conductivity with tem-
perature was taken from [12].
2.4. Nucleation model
The classical nucleation theory (CNT) was used to model homo-
geneous nucleation. The rate of the steady state nucleation was calcu-
lated at each time step by Eq. (5) [13]:
4ν 2/3 ΔG −ΔG∗
I ss = nc exp [ ] ment with experiments [14]. The nuclei are grown gradually and finally
Vm 2/3 6πnc kB T kB T (5)
where, ν = kB T /3πλ2μ is the molecular jump frequency, µ is visc-
osity, λ is the diffusional jump distance, nc = 32πγ 3/3ΔG is the number
of molecules in a critical nucleus, ΔG* is the nucleation barrier, i.e.,
ΔG*= 16πγ 3/3ΔG 2 , Vm is the molecular volume , and kB is the
Boltzmann constant. Note that the transient nucleation rate was ignored
in our model due to the fast kinetics of PT. Based on the steady state
nucleation rate, Eq. (5), the nucleation probability, PN, can be calcu-
lated as:
PN = 1 − exp(−I ssΩA Δt )
(6)
where Δt is the time step (10 ns), and ΩA is the volume of the
-2
amorphous phase. Eq. (6) shows a reduction in the nucleation prob-
ability as the amorphous phase gradually is transformed to the crys-
talline phase. A separate subroutine, i.e., an explicit nucleation algo-
rithm, was written to introduce a nucleus with critical size to the
system. In this algorithm, a new critical nucleus with a radius of r* was
introduced to the system according to the probability of nucleation. The
explicit nucleation algorithm can be found in [8]. Also, Fig. 2 shows the
simulation flowchart of the model and interaction among several
5
Journal of Crystal Growth 542 (2020) 125687
subroutines.
2.5. Growth velocity
The velocity of crystal growth is required to determine the kinetic
coefficient in the phase-field approach, Section 2.1. The generic form of
the velocity of crystal growth was selected to cover the range of the
operating temperature.
4ratom ∙kB T 1 ΔG (T )
VG (T ) = ∙ ∙ [1 − exp(− )]
3πλ2Rhyd μ (T ) kB T (7)
where ratom is the atomic radius, Rhyd is the hydrodynamic radius, µ is
viscosity, and λ is the diffusional jump distance. It is worth noting that
Eq. (7) underestimates the growth velocity for T < 543 K, however
nucleation is dominant in this temperature range and crystal growth is
negligible. So, implementing classical growth velocity does not have
drastic effect on the results.
A viscosity model based on ultra-fast measurement techniques [9]
was used in our model.
log10 μ (T )
Tg m Tg
= log10 μ∞ + (12 − log10 μ∞ ) × exp[( − 1)( − 1)]
T 12 − log10 μ∞ T
(8)
wheremandμ∞ are material constants. All of the constants are
summarized in Table 1.
3. Results and Discussion
3.1. Isothermal annealing
The crystallization of a-GST follows the
Johnson–Mehl–Avrami–Kolmogorov (JMAK) equation, i.e.,
X (t ) = 1 − exp(−bt n ) , where n = 4, and b = (1/3) πVG3 I ss are material
constants [8]. To verify the theoretical model that was presented, the
isothermal annealing of a-GST at T = 463 K, and 488 K was simulated,
and the results were compared with the JMAK model, Fig. 3a. The PF
results follow the JMAK model despite the fact that no new fitting
parameters were used in our proposed PF model. Note that, in the
isothermal model, only the PF model was solved, and the temperature
was constant during the simulation. Fig. 3b-d show the nucleation/
growth during the crystallization process. An incubation time of 12 s is
required for nucleation at T = 463 K which is reduced to 0.3 s for
T = 488 K. The decrease in incubation time is qualitatively in agree-
conglomerate to complete the crystallization. This model can be used to
study the data retention of PCMs at various temperatures.
3.2. Set process
In the set process, the a-GST film was exposed to a constant external
voltage of 0.5 V to raise its temperature above Tg and consequently
trigger the crystallization process. Fig. 4 shows the temperature profile
and phase distribution at various times. The temperature of the film
rapidly reached an almost homogenous temperature distribution due to
the large thermal resistivity at the boundaries and its thinness; the
temperature difference between the hot and cold zones is 1 K (right
color code in Fig. 4a), which is negligible in comparison to the oper-
ating temperature of the device, which ranges from Tg to Tm. The heat
conduction characteristic time is proportional to square of system
length, (Δl)2 . So, an increase in the thickness of the film (increasing the
characteristic time) or a decrease in the thermal resistivity at the
boundaries (reducing the temperature at boundaries) generates more
heterogeneity in the thermal distribution, i.e., the maximum tempera-
ture occurs at the center, and the temperature decreases gradually
H. Attariani, et al.
Fig. 6. Progress of crystallization and the temperature distribution in the Set process for an 0.8-V pulse voltage: a) Applied pulsed voltage vs. time; b-f) crystal
temperature distribution at t = 18.5, 23.1, 28.5, 35, and 30.8 ns. The structural order parameter is varying between 0 and 1 and is shown by the eta symbol on the
corresponding color legend.
toward the boundaries due to the dissipation of the heat into the
electrodes. In this scenario, the presence of thermal gradient makes it
necessary to include the thermoelectric effects. The first crystal nucleus
appeared at T = 445 K, which was less than Tg, and the second nu-
cleation event occurred at T = 477 K, which is greater than Tg. How-
ever, Fig. 4 shows that a high concentration of nuclei occurred at
T = 560 K (Fig. 4c), which corresponded to the maximum nucleation
rate (Fig. 5). Note that, due to the small growth velocity (Fig. 5), the
nuclei did not grow significantly up to this stage. However, the growth
of the nuclei becomes visible when the temperature increases above
600 K (Fig. 4d). In this stage, due to the contrast between the thermal
properties of the amorphous phase and the crystalline phase, the tem-
perature distribution of the cell becomes slightly heterogeneous, i.e.,
the c-GST has smaller heat capacity and larger thermal conductivity
than a-GST. This phenomenon also can be related to the latent heat of
crystallization. The free energy of a-GST is higher than its crystalline
counterpart. So, the transition from the amorphous phase to the crys-
talline phase is accompanied by releasing the latent heat of
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Journal of Crystal Growth 542 (2020) 125687
crystallization, which, consequently, results in an additional increase in
temperature of the cells. This heat is localized at the crystal-amorphous
interface, and it induces a self-heated zone [7], which leads to addi-
tional increase in temperature (Fig. 4c-d). Generally, there are two
distinct regimes in the crystallization of GST, i.e., the nucleation-
dominant region between 445 and 600 K and the growth-dominant
zone, which becomes significant above 600 K. These zones are shown in
Fig. 5 based on Eqs. (5) and (7). So, the final microstructure of the
crystal phase can be controlled by controlling the heating rate. A slow
heating rate allows the material to spend more time in the nucleation
zone, which results in fine grains. In contract, a fast heating rate leads
to a large grain structure since fewer nuclei are formed in the nuclea-
tion region, and crystal growth is dominant. This observation was in
agreement with experimental results [5].
To better understand the self-heating mechanism, a pulse voltage
with an intensity of 0.8 V was applied for 28 ns to trigger crystal-
lization, and then it was removed (Fig. 6a). The central hypothesis in-
volves self-sustaining crystallization even without applying any
H. Attariani, et al.
external voltage and only due to the release of latent heat of crystal-
lization and the confinement of heat in the cell. In this scenario, the
average temperature of the cell reached 716 K in 28 ns, and the crys-
tallization continues even after turning off the voltage. Also, the tem-
perature rises to 880 K as more a-GST is converted to c-GST due to self-
heating mechanism. This finding provided a fresh perspective on the
crystallization mechanism of PCMs. Designing a cell with adequate
thermal confinement to take advantage of the released latent heat can
lead to the fabrication of more efficient memory drives with larger bit-
capacities, i.e. a small external voltage is required to complete the set
process.
4. Conclusion
A thermodynamically-consistent multi-physics model was devel-
oped to study the crystallization of a-GST nano-film. The model that
was presented was in good agreement with JMAK formalism. During
the crystallization, additional heat was released, leading to self-heating
of the cell and an additional increase in temperature. A pulsed voltage
was added to the thin film to determine the effect of self-heating on the
growth of crystal. It was observed that, even after removing the voltage,
the nuclei grew due to the confinement of heat in the cell and also the
release of the latent heat of crystallization. These findings show the
importance of thermal management in designing efficient PRAMs. In
the future, the heterogeneous nucleation model can be added to this
framework to model the effect of the interface on the nucleation. Also,
the implemented Helmholtz free energy can model the GST melting
reset process, since it represents the crystal instability above its melting
point. Another potential application of this coupled model would be
simulating the entire PCRAM architecture to better understand the
behaviors of the system.
Declaration of competing interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influ-
ence the work reported in this paper.
Acknowledgments
The support of Wright State University is gratefully acknowledged.
Also, the authors would like to thank Ohio Super Computing (OSC),
Grant No. ECS- PWSU0463, and Dr. K. Momeni, Louisiana Optical
Network Initiative (LONI),USA for providing the computational re-
sources.
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