Ultrasonics - Sonochemistry 70 (2021) 105307

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Ultrasonics - Sonochemistry
journal homepage: www.elsevier.com/locate/ultson

The Gilmore-NASG model to predict single-bubble cavitation in T

compressible liquids
Fabian Denner
a
Chair of Mechanical Process Engineering, Otto-von-Guericke-Universität Magdeburg, Universitätsplatz 2, 39106 Magdeburg, Germany

ARTICLE INFO ABSTRACT

Keywords: The Gilmore model is combined with the Noble-Abel-stiffened-gas (NASG) equation of state to yield a simple
Cavitation model to predict the expansion and collapse of spherical bubbles based on real gas thermodynamics. The NASG
Bubble dynamics equation of state resolves the temperature inaccuracy associated with the commonly employed Tait equation of
Rayleigh-Plesset models state for liquids and, thus, can provide a consistent description of compressible and thermal effects of the bubble
Real gas
content and the surrounding liquid during cavitation. After a detailed derivation of the proposed Gilmore-NASG
model, the differences between the classical Gilmore-Tait model and the proposed model are highlighted with
results of single-bubble cavitation related to bubble collapse and driven by an acoustic excitation in frequency
and amplitude regimes relevant to sonoluminescence, high-intensity focused ultrasound and shock wave li-
thotripsy. Especially for rapidly and violently collapsing bubbles, substantial differences in the bubble behaviour
can be observed between the proposed Gilmore-NASG model and the classical Gilmore-Tait model. The ability of
the Gilmore-NASG model to simultaneously predict reliable pressure and temperature values in gas, vapour and
liquid, makes the proposed model particularly attractive for sonochemistry and biomedical applications.

1. Introduction During the expansion and collapse of a bubble, heat is exchanged

between the gas (or vapour) inside the bubble and the surrounding li-
The Rayleigh-Plesset (RP) model [1] and its various extensions are quid as a result of thermal diffusion as well as evaporation and con-
the workhorse of theoretical studies of bubble dynamics and cavitation. densation [14]. The liquid, thus, regulates the temperature of the
All RP models have in common that (i) the modelled bubble dynamics bubble content, whereby the large heat capacity of the liquid plays a
are spherical and that (ii) the compression and expansion of the gas or dominant role [15]. Representing the heat capacity of the liquid sur-
vapour inside the bubble is a polytropic process. Yet despite these rounding the bubble accurately, therefore, has a direct influence on the
seemingly limiting simplifications, RP models have been very successful temperature and, in turn, on the pressure and chemical reactions inside
in modelling a broad range of bubble dynamics and cavitation phe- the bubble.
nomena [2]. Among the various extensions of the RP model to include A conceptually simple model to predict the expansion and collapse
the compressibility of the liquid or soft matter surrounding the bubble of spherical bubbles based on a consistent EOS for both the gas or va-
[3,4], the model proposed by Gilmore [5] is generally considered one of pour inside the bubble as well as the liquid surrounding the bubble is
the most widely applicable models [2,6]. not available to date. In order to remedy this shortcoming, a Gilmore
The Gilmore model is traditionally founded on the Tait equation of model based on the Noble-Abel-stiffened-gas (NASG) EOS is proposed.
state (EOS), the polytropic form of the stiffened-gas EOS [7], to describe The NASG EOS is able to describe both compressible and thermal effects
the liquid. While the Tait EOS is able to represent the compressibility of in gases, liquids and their vapours reliably using a single EOS [8,9,16].
common liquids, such as water, accurately, it fails to predict their
temperature [8,9], due to an unphysically large polytropic exponent 2. Noble-Abel-stiffened-gas equation of state
and underpredicted heat capacity. This is a significant shortcoming for
applications in which an accurate prediction of the bubble behaviour as The NASG EOS [8] combines the stiffened-gas EOS and the Noble-
well as the temperature and the pressure of the liquid is critical, such as Abel EOS to yield an unconditionally convex EOS that includes both
sonochemistry [10], sonocrystallisation [11] or ultrasound-based molecular attraction and repulsion. The original idea for the NASG EOS
medical treatments [12,13]. goes back to Tammann [17], as studiously pointed out by Radulescu

E-mail address: [email protected].

https://doi.org/10.1016/j.ultsonch.2020.105307
Received 21 May 2020; Received in revised form 13 July 2020; Accepted 7 August 2020
Available online 20 August 2020
1350-4177/ © 2020 Elsevier B.V. All rights reserved.
F. Denner Ultrasonics - Sonochemistry 70 (2021) 105307

[9]. Rref 3
= ,
The NASG EOS is defined by its thermal and caloric equations of G g,ref
R (11)
state, which are given as [8]
where Rref is the reference bubble radius and g,ref is the associated gas
( 1) c v T density. The pressure of the gas in the bubble is then given, following
p (v , T ) = B
v b (1) Eq. (6), as

( 1) (e q) G (1 bg g,ref )
g
p (v , e ) = B pG = (pg,ref + Bg ) Bg ,
v b (2)
g,ref (1 bg G) (12)
respectively, where p is the pressure, T is the temperature, e is the
specific internal energy, v is the specific volume, b is the co-volume that where subscript g denotes the properties of the gas and pg,ref is the
represents the volume occupied by the individual molecules, B is a predefined reference gas pressure associated with Rref . The pressure in
pressure constant that models molecular attraction, is the heat ca- the liquid at the bubble wall is defined as [2]
pacity ratio, c v is the heat capacity at constant volume and q is a specific 2 R
reference energy. For a fluid modelled by the NASG EOS, the speed of pL = pG 4µ ,
R R (13)
sound is
where is the surface tension coefficient and µ is the dynamic visc-
p+B osity of the liquid. The liquid speed of sound at the bubble wall follows
c= ,
(1 b ) (3) from Eq. (3) as

where = 1/ v is the density, and the enthalpy is pL + B

CL = ,
h= c v T + b p + q. (4) L (1 b L) (14)

Along the isentrope, the NASG EOS yields [9] where subscript denotes the properties of the liquid and

(5)
1
(p + B ) ( v b) = const. K (p L + B )
L = 1
By replacing the heat capacity ratio with the general polytropic 1 + b K (pL + B ) (15)
exponent , the isentropic relation given in Eq. (5) is readily turned into
a polytropic NASG EOS, given as [18] is the density of the liquid at the bubble wall, with the constant re-
1
presenting the liquid reference state given as
= K (p + B ) ,
1 b (6) K =
,ref
,
1
where K is a constant representing the reference state, (p ,ref + B ) (1 b ,ref ) (16)

K= ref
, where p ,ref and ,ref are the predefined reference pressure and re-
(pref + B ) (1
1
b (7) ference density of the liquid, respectively. The enthalpy difference
ref )
H = hL h is given, based on Eq. (8), as
with pref and ref the predefined reference pressure and reference den-
sity, respectively. The enthalpy of a polytropic NASG fluid follows by pL + B p +B pL p
H= b ,
inserting Eq. (1) into Eq. (4) as 1 L 1 (17)
p+B b where
h= (p + B ) + b p + q,
1 1 (8)
p = pL,0 + pa (18)
and the temperature of this polytropic process follows by inserting Eq.
(1) into Eq. (5) as is the pressure of the liquid at infinity, with pL,0 the ambient pressure in
the liquid and pa the acoustic excitation pressure, and
1
p+B 1
T = Tref . K (p + B )
pref + B (9) = 1
1 + b K (p + B ) (19)
Conveniently, the NASG EOS readily reduces to the Tait EOS
(b = 0, B > 0 ), the ideal-gas EOS (b = 0, B = 0 ) or the Noble-Abel is the corresponding density at infinity. The derivative of H readily
EOS (b > 0, B = 0 ), dependent on the chosen fluid parameters. follows as

3. Gilmore-NASG model H = 1
pL + B
L ( pL
pL + B
L
L )
The Gilmore model [5] describes the temporal evolution of the
p +B
( p
p +B ) b
pL p
1
,
(20)
bubble radius R by a second-order ordinary differential equation, given
as where the derivatives of pressure are

R 3 R R R H p = pa (21)
1 R R¨ + 1 R2 = 1 + H+ 1 R ,
CL 2 3 CL CL CL CL (10)
2 R2 R¨
pL = pG + R + 4µ
where CL is the speed of sound of the liquid at the bubble wall and H is R2 R2 R (22)
the difference between the enthalpy of the liquid at the bubble wall and
at infinity. Combining the Gilmore model, Eq. (10), with the NASG EOS, G g (pG + Bg )
thus, requires suitable definitions for CL and H. pG =
G (1 bg G) (23)
The density of the gas in the bubble follows from the conservation of
mass as and the derivatives of density are

2
F. Denner Ultrasonics - Sonochemistry 70 (2021) 105307

p
= (1 b )
(p + B ) (24)

pL L
L = (1 b L)
(pL + B ) (25)

R
= 3 .
G G
R (26)

Inserting the expressions for and L into Eq. (20) simplifies the
derivative of the enthalpy difference to
pL p
H= .
L (27)

Extending existing models based on the original formulation of

Gilmore [5] to the improved formulation proposed above, merely re-
quires to amend the definitions of density, pressure, speed of sound and
enthalpy, as described in this section. The implementation of the Gil-
more-NASG model is discussed in Appendix A.

4. Results
Fig. 2. Evolution of the bubble radius R, as well as the gas temperature TG and
liquid temperature TL(r = R) at the bubble wall during the first collapse, predicted
To highlight the differences between the classical Gilmore-Tait
by the Gilmore-Tait model and the Gilmore-NASG model for a bubble with
model and the proposed Gilmore-NASG model, the results of four re- R 0 = 3 µ m driven by an acoustic excitation with pa = 135 kPa and fa = 25 kHz .
presentative cavitation events of an air bubble in water are presented.
The system of ordinary differential equations arising from Eq. (10), see
Eqs. (A.11) and (A.12) in Appendix A, is solved using a fourth-order 4.2. Sonoluminescence
Runge–Kutta method with adaptive time-stepping [19]. Air is described
with g = 1.4, Bg = 0 and g,ref = 1.2 kg/m3 , and bg = 0 unless stated The cavitation of a bubble with initial radius R 0 = 3 µm driven by a
sinusoidal acoustic excitation defined as
otherwise. Water has the properties = 1.19, B = 6.2178 × 10 8 Pa ,
b = 6.7212 × 10 4 m3/kg and ,ref = 997 kg/m3 [20] for the NASG EOS pa = pa sin(2 fa t ), (28)
and = 7.15, B = 3.046 × 108 Pa and ,ref = 997 kg/m3 for the Tait
EOS. In all cases, the reference pressure is pg,ref = p ,ref = 105 Pa . The with pressure amplitude pa = 135 kPa and frequency fa = 25 kHz is
reference temperature, which is not required to solve Eq. (10) and is considered next, an acoustic regime relevant for sonoluminescence
defined only for post-processing, is Tref = 300 K . Since thermal transport [21]. The bubble is initially in equilibrium, with pG,0 = pL,0 + 2 / R0
(advection, diffusion and radiation) and mass transfer are neglected, and pL,0 = 105 Pa . The viscosity of the liquid is µ = 0.001 Pa s and the
the liquid temperatures given below likely represent an upper limit. surface tension is = 0.072 N/m . The evolution of the bubble radius R is
shown in Fig. 2, alongside the gas temperature TG and the liquid tem-
perature TL(r = R) at the bubble wall during the first collapse. While the
4.1. Rayleigh collapse
temperature in the liquid at the bubble wall differs significantly for
both models, the evolution of the radius exhibits only very small dif-
First, a simple Rayleigh collapse of a bubble with initial radius
ferences between the two models. Interestingly, the temperature pre-
R 0 = 1 m is considered, induced by an overpressure in the liquid at
dicted in the liquid by the Gilmore-Tait model is higher than the cor-
infinity of p = 105 Pa against the initial gas pressure pG,0 = 10 4 Pa in
responding gas temperature, a physically questionable result.
the bubble. Viscosity and surface tension are neglected. Fig. 1 shows the
evolution of the bubble radius R and the temperature TL(r = R) , obtained
via Eq. (9), of the liquid at the bubble wall. While the bubble radius is in 4.3. High-intensity focused ultrasound
excellent agreement for both Gilmore models, the Gilmore-Tait model
predicts a significantly higher temperature in the liquid. This is a The application of ultrasound-based diagnostic and therapy
manifestation of the unphysically large polytropic exponent of the Tait methods in biomedical applications requires an accurate prediction of
model ( 7 ), chosen to approximate the compressibility of the liquid. the peak pressure amplitudes and the heat generated in the surrounding
blood or tissue [12,22]. Fig. 3 shows the behaviour of a bubble with
R 0 = 1.25 µm and = 0.072 N/m driven by a sinusoidal acoustic ex-
citation, Eq. (28), with pa = 1.25 MPa and fa = 750 kHz , which is ty-
pical for high-intensity focused ultrasound treatments [23]. The visc-
osity of the liquid is µ = 0.001 Pa s and the bubble is initially in
equilibrium, with pL,0 = 105 Pa . The Gilmore-NASG model predicts a
stronger collapse of the bubble than the Gilmore-Tait model, with a
smaller minimum bubble radius and a considerably higher peak velo-
city of the bubble wall. However, the peak Mach number of the bubble
wall, ML = U / CL , is similar with both models, since the Gilmore-NASG
model also predicts a higher pressure and, consequently, a larger speed
of sound of the liquid due to the stronger collapse of the bubble. In both
Fig. 1. Bubble radius R and liquid temperature TL(r = R) at the bubble wall as a cases the Mach number stays below 2.2 , the upper bound of validity
function of dimensionless time t / t c , with tc = 0.915 R 0 / p the Rayleigh previously proposed for the Gilmore model [5]. The Gilmore-Tait model
collapse time, predicted by the Gilmore-Tait model and the Gilmore-NASG again predicts a peak temperature of the liquid at the bubble wall that
model for the Rayleigh collapse of a bubble with R 0 = 1 m and p / pG,0 = 10 . exceeds the gas temperature.

3
F. Denner Ultrasonics - Sonochemistry 70 (2021) 105307

Fig. 3. Evolution of the bubble radius R, the velocity U and Mach number U / CL of the bubble wall, and the temperature of the gas TG and the liquid TL(r = R) at the
bubble wall, predicted by the Gilmore-Tait model and the Gilmore-NASG model for a bubble with R 0 = 1.25 µm driven by an acoustic excitation with pa = 1.25 MPa
and fa = 750 kHz .

Fig. 4. Evolution of the bubble radius R, the velocity U and Mach number U / CL of the bubble wall, and the temperature of the gas TG and the liquid TL(r = R) at the
bubble wall, predicted by the Gilmore-NASG model with bg = 0 and bg = 10 3 m3/kg for a bubble with R 0 = 1.25 µm driven by an acoustic excitation with
pa = 1.25 MPa and fa = 750 kHz .

The cases presented above neglect the co-volume of the gas, bg , in [8]. The NASG equation of state provides a consistent description of
the NASG model. However, especially for inertial cavitation, where the compressible and thermal effects of both gases and liquids, resolving
gas in the bubble is compressed very strongly and rapidly, the volume the temperature inaccuracy associated with the commonly used Tait
occupied by the individual gas molecules becomes an important factor. equation of state. Even without considering thermal diffusion and mass
Fig. 4 shows the same cavitation event as Fig. 3, now using the Gilmore- transfer, which both play an important role in the dynamic behaviour of
NASG model with bg = 10 3 m3/kg , an approximate value typical for cavitation bubbles [14] but have not been considered in the presenta-
gases [24], compared against bg = 0 . The non-zero co-volume of the gas tion of the proposed model, significant differences in the bubble be-
inhibits the collapse markedly, with a considerably reduced peak ve- haviour can be observed between the proposed Gilmore-NASG model
locity of the bubble wall. The Mach number of the bubble as well as the and the classical Gilmore-Tait model, especially for rapidly and vio-
temperatures of the gas and the liquid, however, do not change sig- lently collapsing bubbles. For the bubbles in the excitation regimes
nificantly. representative of high-intensity focused ultrasound and shock wave li-
thotripsy treatments, the velocity of the bubble wall predicted by the
4.4. Shock wave lithotripsy Gilmore-NASG model is approximately twice as high as the velocity
predicted by the Gilmore-Tait model, a difference that may be im-
Following the work of Church [25], a shock-driven bubble collapse portant for clinical safety considerations of such treatments [13].
representative of shock wave lithotripsy treatments is considered. The The ability of the Gilmore-NASG model to predict pressure and
bubble collapse is driven by a shock wave, defined as [25] temperature values in gas, vapour and liquid simultaneously, makes the
proposed model particularly attractive for sonochemistry and biome-
pa = 2 pa e t cos 2 fa t + , dical applications. While an accurate description of evaporation and
3 (29) condensation together with a consistent model of the vapour inside the
with fa = 83.3 kHz, pa = 10 MPa and the decay constant = 910 kHz . bubble are key to predict and understand chemical reactions occurring
The bubble has an initial radius of R 0 = 9 µm and is initially in equili- inside the bubble [26–28], the temperature distribution and the accu-
brium, with pL,0 = 105 Pa . The liquid has a viscosity of mulation of heat in the liquid are primary concerns with respect to the
µ = 0.001 Pa s and the surface tension is = 0.072 N/m . The bubble efficacy and safety of medical treatments [12,22,13]. All these phe-
behaviour, shown in Fig. 5, exhibits similar differences between the nomena necessitate an accurate temperature prediction in the liquid.
classical Gilmore-Tait model and the proposed Gilmore-NASG model as The Gilmore-NASG model can, therefore, serve as the foundation for
the bubble considered in Section 4.3; the peak velocity of the bubble future model developments, e.g. for supercritical fluids [16] in so-
wall predicted by the Gilmore-NASG model is considerably higher and nochemistry applications, and studies related to cavitation events in
the Gilmore-Tait model yields a higher peak temperature in the liquid which an accurate knowledge and consistent definition of pressure and
than in the gas. temperature of the liquid are critical, such as sonocrystallisation [11]
and medical ultrasound applications [12].

5. Conclusions
CRediT authorship contribution statement
A new model for the prediction of single-bubble cavitation in
compressible liquids has been presented, by combining the Gilmore Fabian Denner: Conceptualization, Methodology, Resources,
model [5] and the Noble-Abel-stiffened-gas (NASG) equation of state Software, Validation, Investigation, Writing - original draft, Writing -

4
F. Denner Ultrasonics - Sonochemistry 70 (2021) 105307

Fig. 5. Evolution of the bubble radius R, the velocity U and Mach number U / CL of the bubble wall, and the temperature of the gas TG and the liquid TL(r = R) at the
bubble wall, predicted by the Gilmore-Tait model and the Gilmore-NASG model for a bubble with R 0 = 9 µm driven by a shock wave with pa = 10 MPa, fa = 83.3 kHz
and = 910 kHz .

review & editing, Funding acquisition. influence the work reported in this paper.

Declaration of Competing Interest Acknowledgements

The authors declare that they have no known competing financial This research was funded by the Deutsche Forschungsgemeinschaft
interests or personal relationships that could have appeared to (DFG, German Research Foundation), Grant No. 441063377.

Appendix A. Implementation of the Gilmore-NASG model

Implementing a Gilmore model to predict the behaviour of a bubble in a viscous fluid requires to rearrange Eq. (10), since the derivative of the
liquid pressure at the bubble wall, pL , and, in turn, the derivative of the enthalpy difference, H , are a function of the acceleration of the bubble wall,
R̈ , which is the primary solution variable. First, defining the coefficient

R
A= 1 R,
CL (A.1)
inserting it in Eq. (10) and rearranging for R̈ leads to

R¨ =
(1 + ) H (1
R
CL
3
2
R
3 CL )R 2

+
H
.
A CL (A.2)
The derivative of the liquid pressure at the bubble wall, pL , defined in Eq. (22), is split into an explicitly treated part and an implicitly treated
part, given as
pL = pL,e + pL,i , (A.3)
with the explicitly treated part defined as

2 R2
pL,e = pG + R + 4µ 2
R 2 R (A.4)
and the implicitly treated part is constituted by the term including R̈ and defined as
R¨
pL,i = 4µ .
R (A.5)
Splitting the enthalpy derivative, see Eq. (27), into explicitly and implicitly treated parts in a similar fashion, follows as
H = He + Hi (A.6)
with
pL,e p
He =
L (A.7)
and
pL,i µ R¨
Hi = = 4 .
L LR (A.8)
Inserting Eqs. (A.7) and (A.8) into Eq. (A.2) and rearranging for R̈ yields
R 3 R
1+ H 1 R2
CL 2 3 CL He
A
+ CL
R̈ =
B (A.9)
with

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F. Denner Ultrasonics - Sonochemistry 70 (2021) 105307

µ
B=1+4 .
L R CL (A.10)
A system of two first-order ordinary differential equations can then be readily defined based on Eq. (A.9) as
R=U (A.11)
U 3 U
1+ H 1 U2
CL 2 3 CL He
A
+ CL
U= ,
B (A.12)
which may be solved with any common ODE solver.

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