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Journal of Non-Crystalline Solids 486 (2018) 27–35

Contents lists available at ScienceDirect

Journal of Non-Crystalline Solids


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

Characterization of glass viscosity with parallel plate and rotational T


viscometry
Youngnam Songa, Chanhee Wona, Seong-hoon Kangb, Howon Leeb, Sung-Jun Parkc,

Sung Hyuk Parkd, Jonghun Yoona,
a
Department of Mechanical Engineering, 55 Hanyangdaehak-ro, Sangnok-gu, Ansan-si, Gyeonggi-do 15588, Republic of Korea
b
Materials Deformation Department, Korea Institute of Materials Science, 797 Changwondaero, Seongsan-gu, Changwon-si, Gyeongnam-do 51508, Republic of Korea
c
Department of Mechanical Engineering, Chungju National University, 72 Daehak-ro, Chungju, Chungcheongbuk-do 27136, Republic of Korea
d
Material Science and Engineering, Kyungpook National University, 80 Daehakro, Bukgu, Daegu 41566, Republic of Korea

A R T I C L E I N F O A B S T R A C T

Keywords: Glass materials have been applied as insulators during hot extrusion of titanium- and nickel-based alloys to
Glass viscosity reduce the friction and thermal conduction in the Ugine-Séjournet process. In this research, parallel plate vis-
Parallel plate viscometer cometry (PPV) and rotational viscometry (RV) tests were carried out to characterize the viscosity of glass ma-
Rotational viscometer terials such as lead-borate, potassium-lead-silicate, and potassium-sodium-lead-silicate, quantitatively. Herein,
VFT equation
we propose a new equation that can be used to predict an extensive range of viscosities from the softening to the
melting point. This equation demonstrates more accurate predictions compared with the conventional
Vogel–Fulcher–Tamman (VFT), the Avramov&Milchev (AM) and the Mauro-Yue-Ellison-Gupta-Allan (MYEGA)
equations.

1. Introduction between the die and billet via an insulating effect. Shaw [9] mentioned
two major functions of viscous molten glass during hot extrusion; it acts
With increasing interest in aerospace industries and offshore plants, as a hydrodynamic lubricant with very high viscosity and as a thermal
including desalination plants, heat- and corrosion-resistant materials insulator to keep the metal adjacent to the die wall at a sufficiently high
with higher strengths, such as titanium- and nickel-based alloys as well temperature to have low shear strength and exert low friction.
as molybdenum, have been extensively produced via hot extrusion Since glass lubricants have different melting temperatures and
[1–3]. There are several critical processing parameters that can be viscosity characteristics depending on their various constituents, it can
controlled to enhance product quality and efficiency; among these, be difficult to select suitable glass lubricants for different hot extrusion
using an appropriate lubricant to minimize friction between the die and processes. For example, in the Ugine-Séjournet process [6], the form of
workpiece while guaranteeing insulation above 800°C is particularly the glass material (e.g., a powder or solid pad) plays a substantial role.
useful [3–5]. In the middle of the 20th century, Séjournet [6] in- This is the case because glass powders tend to be applied to the outer
troduced a new lubricant made of glass powder, solid lubricants and an surface of the initial billet to reduce friction between the billet and
organic bonding material; this lubricant helped increase tool life sig- extrusion die, while glass pads are installed in front of the entry die as a
nificantly, especially when hot forming high alloys such as nickel, ti- reservoir to provide continuous molten glass lubricant throughout the
tanium alloys, stainless steels, molybdenum, and heat-resisting mate- hot extrusion process [10]. Therefore, it is necessary to examine var-
rials. Li et al. [7] and Udagawa et al. [8] demonstrated that using glass iations in the glass viscosities extensively, from the melting to softening
lubricants in the hot extrusion process for Ti alloys extends die life by points, for the hot extrusion process of high alloys.
preventing excessive die chilling and non-uniform heat conduction Joshi et al. [11] conducted parallel plate viscometry (PPV), which is


Corresponding author.
E-mail address: jyoon@hanyang.ac.kr (J. Yoon).

https://doi.org/10.1016/j.jnoncrysol.2018.02.003
Received 2 January 2018; Received in revised form 1 February 2018; Accepted 6 February 2018
0022-3093/ © 2018 Elsevier B.V. All rights reserved.
Y. Song et al. Journal of Non-Crystalline Solids 486 (2018) 27–35

a standard test used to obtain glass viscosities in the range of parallel plates moving perpendicular to their common central axis, as
104 Pa·s ≤ η ≤ 108 Pa·s. They suggested that PPV can be extended to depicted in Fig. 1 [17]. This apparatus consists of a balancing weight,
measure viscosities above 108 Pa·s, as long as the friction coefficient is load bar, linear variable differential transformer (LVDT), 500-g load,
known for the glass/mold combination at the temperature of interest; and heating chamber (used to control the holding temperature and
beam bending viscometry (BBV) is not necessary. Bouchard et al. [12] heating rate). The initial glass pad, which has a diameter of 12 mm and
proposed a new lubricant-trapping thermomechanical test to identify height of 4.25 mm, is placed on the alumina plate. At the initial setting,
the thermomechanical behavior of glass lubricants under different the 500-g load is put on a plate at the top of the load bar after the total
temperature and strain rate conditions; this allows the identification weight of the load bar and upper plate has been offset completely by the
procedure to be carried out under thermomechanical conditions that balancing weight; this guarantees that only the actual weight of a load
are as close as possible to industrial conditions. Yan [13] and Jain [14] is applied to the glass pad in the heating process. As shown in Fig. 1, the
measured glass viscosity near the softening point using parallel plate LVDT precisely measures the displacement of the balancing weight as
viscometry testing; these results were fitted with the Vogel–Ful- the temperature increases to the target temperature at a constant rate of
cher–Tamman (VFT) equation to demonstrate variations in the viscosity 5°C/min [17]. The balancing weight tends to move upward during the
with respect to temperature. Kobayashi et al. [15] examined the visc- heating process because the initial glass pad loses its resistance to the
osity behaviors of organic and inorganic glasses with a rotational applied load when it is transformed into a softened glass. The wire
viscometer (RV); they measured viscosities between 10−1 and 108 Pa·s. tends to be influenced substantially by friction in the pulley when it is
Hagy [16] compared the viscosity data of a soda-lime-silica glass that passed through the pulley. While ASTM C1351M-96 [17] utilizes a wire
were collected by both beam-bending and fiber-elongation methods for to connect the balancing weight and the load bar through a pulley, we
a very high range of viscosities. Most previous researches only mea- replaced the wire with a bar (600-mm-long) that was linked through a
sured the glass viscosity for a limited range with a single PPV or RV test; pivot so it would respond to changes in the height of the glass pad with
these findings are typically fitted with the VFT equation to extend the more sensitivity relative to the conventional method.
results to a wider viscosity range via extrapolation. In our study, an To derive theoretical relationships between the viscosity and ex-
exponential viscosity equation has been proposed based on both PPV perimental data, such as the reduction rate in the height of the glass pad
and RV tests. This equation was proven to be accurate over a wide and the reaction force, from the PPV test, the total deformation is as-
range of viscosities for three glass materials (i.e., potassium-lead-sili- sumed to be decomposed into two parts under no-slip and perfect slip
cate, potassium-sodium-lead-silicate, and lead-borate glasses) that have conditions with respect to friction, as depicted in Fig. 2. The corre-
been commonly utilized in the hot extrusion process of high alloys. sponding forces F1 and F2 are calculated in Appendix A. The final ap-
plied load F is calculated by combining F1 and F2 [19–21].

2. Experimental procedure 3Vo (2πh3 + Vo ) dh (t )


F = F1 + F2 = η
2πh5 dt (1)
We prepared three glass materials: lead-borate, potassium-lead-si- −1
Fh5 ⎛ dh (t ) ⎞
licate, and potassium-sodium-lead-silicate. These glasses are referred to η = 2π
3V0 (2πh3 + V0 ) ⎝ dt ⎠ (2)
as LB, PLS, and PSLS, respectively, and their compositions are shown in
Table 1. Their viscosity was measured quantitatively. The rotational viscometer (RV) is another device used to measure
Parallel plate viscometry (PPV) test (ASTM C1351M-96 [17]) is the relatively low viscosities around the melting temperature of a glass
typically utilized to measure glass viscosity (η) between 104 and material, from approximately 1 (=100) to 106 Pa·s. This is done by
108 Pa·s, which includes the softening point (η ≈ 106.6 Pa·s) of the glass. calculating the torque that is needed to rotate a spindle immersed in the
Alternatively, the rotational viscometry (RV) test (ASTM C965–96 [18]) molten glass at a constant angular velocity [22,23] as shown in Fig. 3.
has been devised to measure the viscosity in the range of RV carried out with a computer-controlled Brookfield rheometer
100 Pa·s ≤ η ≤ 106 Pa·s, which includes the melting point of the glass (model DV-III) where shredded glass, with a diameter ranging from 1 to
(η ≈ 10 Pa·s). Although both experimental setups are theoretically able 5 mm, is placed between the outer cylinder and the inner spindle. The
to measure an extensive range of viscosities, it can be difficult to temperature is then decreased from the melting point of the glass. While
measure the viscosity around the softening point via the RV test be- the PPV test measures the viscosity with increasing temperature (from
cause the abrupt increase in torque is apt to cause damage to the testing room temperature to the softening point), the RV test tends to measure
machine when the glass undergoes phase transformation. Under these the torque under a constant spindle speed with decreasing temperature
circumstances, it is necessary to determine the viscosity distribution (from the melting point); this information is converted to glass viscosity
and make use of a reliable equation that represents the viscosity char- in Appendix B and the final viscosity η in the RV test is expressed as Eq.
acteristics from the melting to softening points; this is aided by using (3) [24].
separate testing approaches, such as the results from PPV and RV
τ T ⎛ 1 1
testing. η= = ⎜ − 2 ⎞⎟
A parallel plate viscometer is an experimental device that can γ̇ 4πLw ⎝ Rs2 Rc ⎠ (3)
measure the viscosity of glass using PPV. This is done by determining
the rate of change in the thickness of a cylindrical specimen between 3. Results and discussion

Table 1
During the PPV test, thermal expansion in each fixture, including
Chemical composition of glass materials (wt%).
the load bar, plate, and lever, can influence the precision of measure-
Glass materials PbO SiO2 Al2O3 B2O3 K2O Na2O MgO ments for the displacement of molten glass as the temperature rises up
to 900 °C. In order to quantify the resultant thermal expansion, vertical
LB 82 5 3 10 – – –
displacements from the LVDT with and without the glass pad were
PLS 58 35 – – 7 – –
PSLS 21 61 – – 6 8 4 compared, as shown in Fig. 4(a). This shows how this variable is af-
fected by thermal expansion during the PPV test. While the level of

28
Y. Song et al. Journal of Non-Crystalline Solids 486 (2018) 27–35

Fig. 1. Schematic diagram for the parallel plate viscometry test.

Fig. 2. Decomposition of deformation in the glass pad under different slip conditions: (a) no-slip condition and (b) perfect slip condition.

displacement continuously increases due to thermal expansion when


the glass pad is not installed, it abruptly decreases at the softening point
(around 520 °C) in the normal PPV test with the glass pad. By excluding
this thermal expansion, the height change in the initial glass pad is
calibrated as depicted in Fig. 4(b), which is converged to the in-
stantaneous dh(t)/dt utilized in Eq. (2). Fig. 5 demonstrates comparison
result between the target heating rate (black solid line) of 5 °C/min
designated in the ASTM C1351M-96 and experimental heating rate in
the current facility as denoted by hollow symbols with three glass
materials (i.e., LB, PLS, and PSLS), which stands for how this current
PPV system is operated, precisely, following the target heating rate. It
should be maintained at 5 °C/min [17] to guarantee stable PPV testing.
Fig. 6(a) demonstrates the distribution of the glass viscosities from 106
to 108 Pa·s based on the PPV tests for LB, PLS, and PSLS. Here, the
reduction rate of viscosity with respect to temperature is largest for LB.
These experimental viscosities are generally extended to the Vogel–-
Fulcher–Tamman (VFT) equation [25–27] to represent a wider range of
viscosity, as expressed in eq. (4), where A is a constant value in-
dependent of the composition, and B and C are adjustable parameters to
Fig. 3. Schematic diagram for the rotational viscometry test. be fitted with applied glass materials [28]. Although the VFT equation

29
Y. Song et al. Journal of Non-Crystalline Solids 486 (2018) 27–35

Fig. 4. Height change in the glass pad with increasing temperature during the PPV test: (a) effect of thermal expansion depending on the installation of a glass pad and (b) height change
in the glass pad.

proposed equation, the number of control parameters was increased


from three (in the VFT equation) to eight.
log η = A0 + A1 e−(T − x 0)/ t1 + A2 e−(T − x 0)/ t2 + A3 e−(T − x 0)/ t3 (5)
Then, a performance test has been conducted with the viscosity
equations between conventional such as Vogel–Fulcher–Tamman
(VFT), Avramov-Milchev (AM) as expressed in Eq. (6), and Mauro-Yue-
Ellison-Gupta-Allan (MYEGA) as expressed in Eq. (7), where A, B and C
are fitting parameters [30–36] and proposed one.
B C
log η = A + ⎛ ⎞
⎝T ⎠ (6)

B C
log η = A + exp ⎛ ⎞
T ⎝T ⎠ (7)
Fig. 8 demonstrates the performance of the proposed equation for
experimental viscosities from both the PPV and RV tests with a cali-
Fig. 5. Heating rate in the PPV test. brated set of control parameters, as shown in Table 3; this equation
demonstrates high quantitative accuracy from the softening to melting
with the optimized coefficients is able to represent experimental data points in terms of the error defined in Eq. (8), as shown in Fig. 9. Here,
locally from 106 to 108 Pa·s, as shown in Fig. 6(b), it cannot be used to n is the number of the experimental data points. Although AM or
guarantee a relatively low viscosity. MYEGA equations are able to predict viscosity distributions compared
with VFT equation with high accuracy, the proposed model improves
B
log η = A + fitting accuracy by 9.93% for LB, 9.79% for PLS, and 7.75% for PLSL as
T−C (4)
shown in Fig. 9.
1
By carrying out the RV tests, the viscosity distribution from 10 to (ηexp − ηfitting )2
n
104 Pa·s was obtained for LB, PLS, and PSLS, as demonstrated in ∑1 ηexp
Fig. 6(c). This was also fitted with the VFT equation for a wide viscosity Errornormalized (%) =
n (8)
range, as shown in Fig. 6(d). It is noteworthy that the extrapolated
viscosity from the fitted VFT equation is able to predict the experi-
mental data, validating its accuracy. Fig. 6(e, f) compares the experi- 4. Conclusion
mental viscosities and fitted data with the VFT equation based on the
PPV (Fig. 6(e)) and RV test results (Fig. 6(f)); this is not able to predict This paper characterizes the viscosity distributions over an ex-
the other experimental viscosities, except for the control points. It is tensive range (from 101 to 108 Pa·s) for three glass materials (i.e., LB,
noteworthy that the VFT equation is unable to provide satisfactory PLS, and PLSL) by carrying out PPV and RV testing; these tests were
predictions for a wide range of viscosities, even when we fit the ex- calibrated with the conventional VFT equation. To improve the accu-
perimental data from both the PPV and RV test results simultaneously, racy of the viscosity equation, a Voce-type equation was proposed for a
as depicted in Fig. 7 and Table 2. wide range of viscosities. This equation improves the prediction accu-
Therefore, it is necessary to propose an advanced equation to re- racy by > 7.75% compared to the MYEGA equation. The main
present the various rates of viscosities with respect to the operating achievements in this study can be summarized as follows:
temperature and specific compositions. To do this, we propose Eq. (5),
which is a Voce-type [29] equation that consists of several exponential 1) In order to carry out the PPV and RV experiments, analytical re-
functions. Here, Ai is a constant that is independent of the compositions lationships between the viscosity and reaction force (based on the
and xi and ti are adjustable parameters. To increase the accuracy of the assumption of a Newtonian fluid) were formulated in detail; these

30
Y. Song et al. Journal of Non-Crystalline Solids 486 (2018) 27–35

Fig. 6. (a) Viscosity distributions for lead-borate (LB), potassium-lead-silicate (PLS), and potassium-sodium-lead-silicate (PSLS) in the PPV test; (b) comparison between the experimental
and fitted data with the VFT equation in the PPV test; (c) viscosity distributions for lead-borate (LB), potassium-lead-silicate (PLS), and potassium-sodium-lead-silicate (PSLS) in the RV
test; (d) comparison between experimental and fitted data with the VFT equation in the RV test; comparison between the experimental and fitted data based on (e) the PPV test and (f) the
RV test.

Table 2
VFT coefficients for the PPV and RV test results.

Glass materials A B C

LB −0.50508 490.37229 587.77852


PLS 0.20356 582.18279 277.63695
PSLS −0.3696 109.04742 1505.76037

were correlated with the experimental results.


2) In the PPV tests, the setup defined in ASTM C1351M-96 was mod-
ified by replacing a pulley with a rigid bar that had a pivot system in
order to minimize the effects of friction.
3) The conventional VFT equation should be fitted with a wide range of
Fig. 7. Comparison between the experimental and fitted data based on both the PPV and viscosities to increase the prediction accuracy.
RV tests, simultaneously.
4) For an extensive range of viscosities from softening to melting

31
Y. Song et al. Journal of Non-Crystalline Solids 486 (2018) 27–35

points, the proposed viscosity equation is able to provide sig-


nificantly more accurate predictions compared to the conventional
VFT, AM and MYEGA equation.

Acknowledgements

This work was supported by a Ministry of Trade, Industry and


Energy (MOTIE) grant funded by the Korean government (no.
N10063269).
This work was also supported by the “Human Resources Program in
Energy Technology” of the Korea Institute of Energy Technology
Evaluation and Planning (KETEP), granted by the Ministry of Trade,
Industry & Energy, Republic of Korea (no. 20174010201310).
The authors have no conflict of interests to declare.

Fig. 8. Comparison between the experimental and fitted data with the proposed equation
using both PPV and RV tests.

Table 3
Coefficients of the proposed equation.

Glass materials x0 A0 A1 A2 A3 t1 t2 t3

LB −283.48 392.46 3.892 5.834 6.656 62.994 1925.41 1936.12


PLS −286.48 556.43 3.092 8.299 8.196 142.744 5757.48 5811.15
PSLS −281.19 611.42 3.034 5.934 5.918 194.634 4099.73 4128.49

Fig. 9. Comparison between the experimental and fitted data with the VFT, the AM, the MYEGA, and proposed equation in PPV and RV tests: (a) for LB; (b) for PLS; (c) for PSLS (d)
Quantitative comparisons of errors between experimental and fitted viscosity models.

32
Y. Song et al. Journal of Non-Crystalline Solids 486 (2018) 27–35

Fig. 10. Cylindrical element of the glass pad extending from one plate to the other [19].

Appendix A

In general, the equation of motion for a Newtonian fluid, when neglecting body forces such as gravity, is given in Eq. (A.1).
∂v 1
ρ + ρ v∙∇v = −∇p + η∇2 v + η∇ (∇∙v)
∂t 3 (A.1)
Here, ρ is the density, v is the velocity, η is the viscosity of the Newtonian fluid, and p is the internal pressure. When the incompressibility
condition of the fluid is assumed, the divergence of the fluid velocity is zero (∇ ∙ v = 0); this is the case because the equation of continuity should be
satisfied. For the slow motion of the incompressible viscous fluid, the ρv ∙ ∇v term in the left-hand side of Eq. (A.1) can be neglected; this produces Eq.
(A.2), which has a simple form:
∂v
ρ = −∇p + η∇2 v
∂t (A.2)
In the cylindrical coordinate system (r, θ, z), Eq. (A.2) is transformed into Eq. (A.3) with boundary conditions (e.g., vθ = 0) due to the circular
symmetry along the θ-direction and vz = 0. This is the case because the fluid velocity along the z-direction is significantly smaller than the fluid
velocity along the r-direction.
∂vr ∂p ∂p 1 ∂ ⎛ ∂vr ⎞ 1 ∂ 2v ∂2vr ⎤
ρ =− + η∇2 vr = − + η⎡ r + 2 2r +
∂t ∂r ∂r ⎢
⎣ r ∂r ⎝ ∂r ⎠ r ∂ θ ∂z 2 ⎥
⎦ (A.3)
In the no-slip condition, i.e., there is no fluid velocity at the interfaces between surface of the parallel plate and upper or lower surface of the glass
pad, the radial velocity, vr, is set to zero at z = 0 and z = h. Then, ∂vr/dz changes rapidly over the thickness h of the glass pad, which makes (1/r) ∙ ∂(r
(∂vr/∂r))/∂r possible to be cancelled out from Eq. (A.3) because ∂vr/dr is negligibly small compared to ∂vr/dz. Additionally, (1/r2) ∙ (∂2vr/∂θ2) is set
to zero due to the symmetry conditions along the θ-direction: ∂vr/dθ = 0. Under steady-state flow, the left-hand side of Eq. (A.3) is assumed to be
zero (i.e., ∂vr/dt = 0), which produces Eq. (A.4).
∂p ∂ 2v
= η 2r
∂r ∂z (A.4)
In order to derive vr from Eq. (A.4), it is integrated twice with respect to z by plugging in the boundary conditions, such as vr = 0 at z = 0 and
z = h, which induces Eq. (A.5).
1 ∂p
vr (z ) = · (z − h) z
2η ∂r (A.5)
It is necessary to correlate Eq. (A.5) with the experimental data (i.e., the fluid pressure p and the height reduction rate dh(t)/dt of the glass pad) to
obtain the viscosity values; these are the only variables to be measured from the PPV test. Furthermore, it is necessary to modify Eq. (A.5) from an
equation that deals with the radial velocity vr to an equation that deals with dh(t)/dt; this can be done by assuming that the reduction in the amount
of flow along the z-direction is equal to the increase in the amount of flow along the r-direction under the assumption for incompressible fluid [19],
as shown in Fig. 10, which yields Eq. (A.6).

dh (t ) ∂ h h3 ∂ ∂p
− dr (rdθ)
dt
= ⎛rdθ
∂r ⎝
∫0 vr dz ⎞ dr = −

dθ ⎛r ⎞ dr
12η ∂r ⎝ ∂r ⎠
12η dh (t ) ∂ ⎛ ∂p ⎞
∴ r= r dr
h3 dt ∂r ⎝ ∂r ⎠ (A.6)

To solve Eq. (A.6), the equation must be integrated twice with respect to r, as demonstrated in Eq. (A.7); here, C and C are integration
coefficients. By plugging in the boundary conditions, such as p = patm at r = R and p = pfinite at r = 0, the final expression for the fluid pressure of the
glass pad can be represented by Eq. (A.8).
3η dh (t ) 2
p= r + C′ ln r + C
h3 dt (A.7)

33
Y. Song et al. Journal of Non-Crystalline Solids 486 (2018) 27–35

3η dh (t ) 2
p=− (R − r 2) + patm
h3 dt (A.8)
The force equilibrium along the z-direction is assured when the reaction force from the glass pad (including the atmospheric pressure) is equal to
the applied load, as defined in Fig. 2(a), which can be used to construct the equality relation shown in Eq. (A.9):
R R
∫0 p2πrdr = F1 + ∫0 patm 2πrdr (A.9)
By inserting Eq. (A.8) into Eq. (A.9), F1 can be expressed in terms of dh(t)/dt, as depicted in Eq. (A.10).
3η dh (t ) 2
R R R
− ∫0h3 dt
(R − r 2)2πrdr +
0

patm 2πrdr = F1 + ∫0 patm 2πrdr
R 3η dh (t )
∴ F1 = −
0

h3 dt
(R2 − r 2)2πrdr
(A.10)
The final expression for the reaction force F1 is obtained by integrating Eq. (A.10) with respect to r, as shown in Eq. (A.11); here, V0 is the initial
volume of the glass pad.
3η V20 dh (t )
F1 =
2πh5 dt (A.11)
Alternatively, in the perfect slip condition, the other applied force (F2) that is used to induce compressive deformation (as depicted in Fig. 2(b)) is
based on the definition of the biaxial extensional viscosity: ηB (=σB / εḂ ). Here, σB is the biaxial stretching stress and εḂ is the biaxial extensional strain
rate. Since the biaxial extensional strain rate is expressed with Eq. (A.12), σB can be derived from Eq. (A.13) by assuming that there is no inertia force
or surface tension of the glass pad, in which R0 is the initial radius and R is the current radius of the glass pad at time t. Therefore, when ηB is equal to
6η for a Newtonian fluid, the biaxial extensional viscosity ηB can be expressed as shown eq. (A.14), which can be further simplified to Eq. (A.15) [20].

dεB dε dh (t ) 1 1 dh (t ) ⎛⎜ε = − 1 ln ⎛ h ⎞ ⎞⎟
εḂ = = B =− , B ⎜ ⎟

dt dh dt 2 h dt ⎝ 2 ⎝ h0 ⎠ ⎠ (A.12)

F2 F h
σB = − = − 22
πR2 πR 0 h 0 (A.13)

2F2h2 ⎛ dh (t ) ⎞−1
ηB =
V0 ⎝ dt ⎠ (A.14)

3ηVo dh (t )
F2 =
h2 dt (A.15)
By integrating Eq. (A.11) and Eq. (A.15), the total applied force under the no-slip and perfect slip conditions is expressed as Eq. (A.16). From this,
the essential relationship between the fluid viscosity and height reduction rate dh(t)/dt is derived as shown in Eq. (A.17) [19,21].
3Vo (2πh3 + Vo ) dh (t )
F = F1 + F2 = η
2πh5 dt (A.16)
−1
Fh5 ⎛ dh (t ) ⎞
η = 2π
3V0 (2πh3 + V0 ) ⎝ dt ⎠ (A.17)

Appendix B

The spindle and crucible axes are set to be concentric in order to utilize the relationship between the shear stress and shear rate (i.e., η = τ / γ ̇),
Here, τ is expressed as shown in Eq. (B.1), r is the radial location where the shear rate is being calculated, T is the torque, and L is the effective length
of the spindle.
L 2π
T= ∫A rτdA = ∫0 ∫0 rτrdθdz = τ ⋅2πr 2L
T
∴τ=
2πr 2L (B.1)
From the Navier-Stokes equation [25], by assuming steady-state flow, Eq. (B.2) can be obtained when the fluid pressure is constant along the r-
direction.
∂ ⎛1 ∂
(rvθ (r )) ⎞ = 0
∂r ⎝ r ∂r ⎠ (B.2)
To derive the solution of Eq. (B.3), it must be integrated twice with respect to r, as shown in Eq. (B.4). Here, C1 and C2 are integration coefficients.
When the spindle rotates at a constant angular velocity of fluid in a crucible that is stationary, the following boundary conditions can be given;
vθ = 0 at r = Rc and vθ = ωRs at r = Rs. By inserting the boundary conditions, the final expression for the velocity in the θ-direction is represented as
Eq. (B.5). Here, Rs is the spindle radius, Rc is the crucible radius, and ω is the angular velocity.
1
rvθ (r ) + C1 r 2 + C2 = 0
2 (B.3)

34
Y. Song et al. Journal of Non-Crystalline Solids 486 (2018) 27–35

vθ (r ) = r ω
( 1
r2

1
Rc2 )
( 1
Rs2

1
Rc2 ) (B.4)

v (r )
ω(r ) = θ =ω
( 1
r2

Rc2
1
)
r
( 1
Rs2

1
Rc2 ) (B.5)
The angular velocity ω(r) at position r can be obtained as shown in Eq. (B.5) (by transforming Eq. (B.4)), and γ̇ can be calculated as shown in Eq.
(B.6) by using Eq. (B.5). Therefore, by integrating the definition of the viscosity and Eq. (B.6), the final viscosity η in the RV test is expressed as Eq.
(B.7).
∂w (r ) 2ω 2ωRc2 Rs2
γ (ṙ ) = r = , ∴ γ̇ =
r 2 (Rc2
− Rs2 )
∂r r2 ( 1
Rs2

1
Rc2 ) (B.6)

τ T ⎛ 1 1
η= = ⎜ − 2 ⎞⎟
γ̇ 4πLw ⎝ Rs2 Rc ⎠ (B.7)

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