J. Phys. Chem.

B 2006, 110, 21145-21151 21145

Modeling the Kinetics of Bubble Nucleation in Champagne and Carbonated Beverages

Gerard Liger-Belair,* Maryline Parmentier, and Philippe Jeandet

Laboratoire dnologie et Chimie Appliquee, UPRES EA 2069, URVVC, Faculte des Sciences de Reims,
Moulin de la Housse, B.P. 1039, 51687 Reims, Cedex 2, France
ReceiVed: June 28, 2006; In Final Form: August 12, 2006

In champagne and carbonated beverages, bubble nucleation was mostly found to take place from tiny Taylor-
like bubbles trapped inside immersed cellulose fibers stuck on the glass wall. The present paper complements
a previous paper about the thorough examination of the bubble nucleation process in a flute poured with
champagne (Liger-Belair et al. J. Phys. Chem. B 2005, 109, 14573). In this previous paper, a model was built
that accurately reproduces the dynamics of these tiny Taylor-like bubbles that grow inside the fibers lumen
by diffusion of CO2-dissolved molecules. In the present paper, by use of the model recently developed, the
frequency of bubble formation from cellulose fibers is accessed and linked with various liquid and fiber
parameters, namely, the concentration cL of CO2-dissolved molecules, the liquid temperature , its viscosity
, the ambient pressure P, the course of the gas pocket growing trapped inside the fibers lumen before
releasing a bubble, and the radius r of the fibers lumen. The relative influence of the latter parameters on the
bubbling frequency is discussed and supported with recent experimental observations and data.

1. Introduction
In champagne and sparkling wines, carbon dioxide molecules
in excess form together with ethanol when yeast ferments sugars.
They are responsible for producing gas bubbles as soon as the
bottle is uncorked. In soda drinks and most of fizzy waters,
industrial carbonation is the source of effervescence.1
Generally speaking, sparkling beverages are weakly super-
saturated with CO2-dissolved gas molecules. In weakly super-
saturated liquids such as carbonated beverages in general, bubble
formation and growth require preexisting gas cavities with radii
of curvature large enough to overcome the nucleation energy
barrier and grow freely.2,3 Jones et al. made a classification of
the broad range of nucleation likely to be encountered in liquids
supersaturated with dissolved gas.4 Bubble formation from
preexisting gas cavities larger than the critical size is referred
to as nonclassical heterogeneous bubble nucleation (type IV
bubble nucleation, following their nomenclature).
The close-up observation of glasses poured with carbonated
beverages recently revealed that most of the bubble nucleation
sites were found to be located on preexisting gas cavities trapped
inside hollow and roughly cylindrical cellulose-fiber-made
structures on the order of 100 m long with a cavity mouth of
several micrometers.5-7 The hollow cavity inside these fibers
where a gas pocket is trapped during the pouring process is
called the lumen. The mechanism of bubble release from a
fibers lumen already has been described and partly modeled
in recent papers.5-8 In short, after a bottle of champagne or
sparkling wine is opened, the thermodynamic equilibrium of
CO2 molecules dissolved in the liquid medium is broken. CO2-
dissolved molecules become in excess in comparison with what
the liquid medium can withstand. Therefore, CO2 molecules will
escape from the liquid medium through every available gas/
liquid interface to reach a vapor phase. Actually, once the
sparkling beverage is poured into a glass, the tiny gas pockets
* Corresponding author. E-mail: gerard.liger-belair@univ-reims.fr.
Tel: (33)3 26 91 86 14. Fax: (33)3 26 91 33 40.
10.1021/jp0640427 CCC: $33.50 2006 American Chemical Society
Published on Web 10/03/2006
trapped inside the collection of fibers adsorbed on the glass wall
offer gas/liquid interfaces to CO2-dissolved molecules, which
cross the interface toward the gas pockets. In turn, gas pockets
grow inside the fibers lumen. When a gas pocket reaches the
tip of a fiber, a bubble is ejected, but a portion of the gas pocket
remains trapped inside the fibers lumen, shrinks back to its
initial position, and the cycle starts again until bubble production
stops through lack of dissolved gas molecules (see Figure 1).
The fiber displayed in Figure 1 is a sort of textbook case, the
behavior of which was recently understood and modeled.8 The
fine mechanisms behind the regular production of bubbles from
those tiny hollow and cylindrical structures are indeed still under
progress.9
Champagne and sparkling wine tasters often pay much
importance to the allure of effervescence in the glass, and even
if there is no evidence yet to believe that bubbles confer any
other sensory advantage to the wine, it often is recognized that
bubbles play a major role in the assessment of champagne and
sparkling wines. For this reason, champagne makers and
champagne houses have spent much effort during the past few
years to better detect, understand, and control the various
parameters involved in the kinetics of effervescence and
foaming. Actually, the average bubbling frequency of a single
cellulose fiber is a key parameter that determines the overall
number of bubbles produced in a glass per second, and,
therefore, the overall kinetics of gas discharging from the
supersaturated liquid.
The model developed in ref 8 accurately reproduces the
dynamics of this tiny Taylor-like bubble that grows inside the
fibers lumen by diffusion of CO2-dissolved molecules. In the
present paper, by use of the model recently developed, the
frequency of bubble formation from cellulose fibers is accessed
and linked with various liquid and fiber parameters, namely,
the concentration cL of CO2-dissolved molecules, the liquid
temperature , its viscosity , the ambient pressure P, the course
of the gas pocket growing trapped inside the fibers lumen before
releasing a bubble, and the radius r of the fibers lumen. The
21146 J. Phys. Chem. B, Vol. 110, No. 42, 2006
Figure 1. (Panels 1-5) Time-sequence illustrating one period of the
cycle of bubble production from the lumen of a typical hollow cellulose
fiber adsorbed on the wall of a glass poured with champagne (reprinted
with permission from ref 8; copyright 2005 American Chemical
Society); the time interval between successive frames is about 200 ms.
Bar ) 50 m.
relative influence of the latter parameters on the bubbling
frequency is discussed and supported with recent experimental
observations and data.
2. Experimental Section
2.1. Material. A standard commercial champagne wine was
poured in a classical crystal flute that was first rinsed using
distilled water and then was air-dried. Some physicochemical
parameters of champagne were already determined at 20 C
with a sample of champagne first degassed.5 The static surface
tension of champagne was found to be on the order of 47
mN/m, its density F was measured and found to be 998 kg/m3,
and its dynamic viscosity was found to be on the order of 1.5
10-3 kg m-1 s-1. In the range of temperature in which
champagne and sparkling wine tasting is concerned (ap-
proximately 5-15 C), their surface tension and density do not
drastically vary. However, in this range of champagne-tasting
Liger-Belair et al.
Figure 2. The champagnes viscosity as a function of temperature in
the range of usual champagne-tasting temperatures (on a semilogarith-
mic scale). The solid line is the best fit to experimental data drawn
with the Arrhenius-like eq 1.
temperatures, the liquid viscosity is highly temperature-
dependent. The temperature dependence of the champagne
viscosity was measured with a thermostated Ubbelhode capillary
viscosimeter. The result is displayed in Figure 2, in which the
champagne dynamic viscosity is plotted vs temperature in the
range of wine-tasting temperatures previously defined. As
expected, the temperature dependence of the dynamic liquid
viscosity (expressed in kg/m/s) accurately follows an Arrhenius-
like equation
() 1.08 10-7 exp(2806/) (1)
where is the absolute temperature (in K).
In a previous work, the carbon dioxide dissolved into the
liquid matrix was accurately measured with an imaging spec-
trometer through use of the 13C magnetic resonance spectroscopy
(MRS) technique, which was an original unintrusive and
nondestructive method.10,11 Typically, champagne holds about
10 g/L of CO2-dissolved molecules (before gas discharging in
a flute). Nevertheless, as time proceeds after pouring this
supersaturated liquid in a flute, the concentration cL of CO2-
dissolved molecules in the liquid progressively decreases to
finally almost vanish a few hours later to fulfill Henrys law,
which states that the concentration of dissolved gas in a solution
is proportional to its partial pressure P in the vapor phase (cL
) kHP, where kH is the Henrys law constant). Actually, like
the dynamic viscosity , kH also is highly temperature-
dependent. Recently, in the case of our standard champagne
wine, the dependence of kH with temperature was expressed
with the following vant Hoff-like equation12
[ )]
Hdiss 1 1
kH() ) k298K exp - (
R 298
- (2)
where k298 K ) 1.21 10-5 kg m-3 ps-1 is the Henrys law
constant at 298 K, Hdiss -24 800 J/mol is the dissolution
enthalpy of CO2 molecules in champagne (in J/mol), and R
is the ideal gas constant (8.31 J mol-1 K-1).
2.2. Set-up Used to Observe Bubble Nucleation in Close-
up. The dynamics of bubble nucleation was captured with a
high-speed digital video camera (Speedcam+, Vannier Photelec,
Antony, France) that was able to film up to 2000 frames per
second and was fitted with a microscope objective (Mitutoyo,
M Plan Apo 5, Japan). The champagne was first poured into
the flute, which was placed between the objective and a cold
source light (Fiber-Lite, PL-900, dc regulated illuminator). A
Kinetics of Bubble Nucleation in Champagne J. Phys. Chem. B, Vol. 110, No. 42, 2006 21147

Figure 3. Scheme (a) and photographic detail (b) of the workbench used to observe bubble nucleation sites in close-up.

scheme of the whole workbench is shown in Figure 3A together

with a photographic detail of the flute emplacement in Figure
3B. The experimental bubbling frequency fexp was directly
accessed simply by measuring the time Texp needed by the
nucleation site to release a bubble (therefore, fexp ) 1/Texp). It
is worth noting that, in the present paper, we focused on
nucleation sites releasing bubbles with clockwork regularity,
which is not always the case. Actually, for a given bubble
nucleation site the time intervals between the release of
successive bubbles may indeed vary. In a previous paper, we
reported some transitions from multiperiodic to single periodic
bubbling regimes during the formation of sparkling bubbles.13
The present paper deals with modeling the bubbling frequency
of nucleation sites that exclusively release bubbles with
clockwork regularity.

3. Results and Discussion

3.1. Required Background. The model developed in a

previous paper that accurately reproduces the dynamics of the
tiny gas pocket, which grows by diffusion inside a fibers lumen
(see Figure 1), is the starting point of our discussion.8
This tiny gas pocket was modeled as a slug-bubble growing
trapped inside an ideal cylindrical microchannel and being fed
with CO2-dissolved molecules diffusing (i) directly from both
ends of the gas pocket and (ii) through the fiber wall, which
consists of closely-packed cellulose microfibrils oriented mainly Figure 4. Real gas pocket trapped inside the lumen of a cellulose
in the direction of the fiber.14 A scheme is displayed in Figure fiber acting as a bubble nucleation site in a glass poured with champagne
(A), which is modeled as a slug-bubble trapped inside an ideal
4 in which the geometrical parameters of the tiny gas pocket
cylindrical microchannel and being fed with CO2-dissolved molecules
growing by diffusion are defined. Taking into account the diffusing (i) directly from the liquid bulk through both ends of the gas
diffusion of CO2-dissolved molecules from the liquid bulk to pocket and (ii) through the wall of the microchannel (B). Bar )
the gas pocket via the two ways defined above, the growth of 50 m.
21148 J. Phys. Chem. B, Vol. 110, No. 42, 2006
Figure 5. Between the release of two bubbles from the fibers tip, the
gas pocket trapped inside the fibers lumen oscillates between two
situations where its length varies from its initial length, denoted z0,
and its final length, denoted zf.
this gas pocket with time t was linked with both liquid and fiber
parameters as follows:
{
z(t) (z0 + A) exp(t/) - A
(P + 2/r)r 4RD0c (3)
with ) , and A )
2RDc (P + 2/r)
where z is the length of the gas pocket, z0 is the initial length
of the gas pocket before it starts its growth through the lumen
at each cycle of bubble production (see Figure 1, panel 1), P is
the ambient pressure, D0 is the diffusion coefficient of CO2-
dissolved molecules in the liquid bulk, D is the diffusion
coefficient of CO2-dissolved molecules through the fiber wall
(and, therefore, perpendicular to the cellulose microfibrils), c
) cL - cB ) cL - kHPB ) cL - kH(P + 2/r) is the difference
in CO2-dissolved concentrations between the liquid bulk and
the close vicinity of the gas pocket surface in equilibrium with
the gaseous CO2 in the gas pocket, and is the boundary layer
thickness where a linear gradient of CO2-dissolved concentration
is assumed.
In a previous work, the transversal diffusion coefficient D
of CO2 molecules through the fiber wall was approached and
was properly bounded by D/D0 0.1 and D/D0 0.3.7 For
modeling purposes, an intermediate value of about D 0.2D0
was proposed and will be used hereafter.
3.2. Modeling the Average Bubbling Frequency. As seen
in Figure 1, the whole process leading to the production of a
bubble from a cellulose fibers tip can be coarsely divided in
two main steps: (i) the growth of the gas pocket trapped inside
the fibers lumen, and (ii) the bubble detachment as the gas
pocket reaches the fibers tip. Actually, it is clear from the
numerous close-up time sequences taken with the high-speed
video camera that the time scale of the bubble detachment is
always very small (1 ms) when compared with the relatively
slow growth of the gas pocket (several tens to several hundreds
of milliseconds). Therefore, the whole cycle of bubble produc-
tion seems to be largely governed by the growth of the gas
pocket trapped inside the fibers lumen. The period of bubble
formation from a single cellulose fiber is therefore equal to the
total time T required by the tiny gas pocket to grow from its
initial length, denoted z0, to its final length, denoted zf, as it
reaches the fibers tip (see Figure 5). By retrieving eq 3, it is
Liger-Belair et al.
possible to access the frequency of bubble formation f from a
single fiber as follows:
1 1
f) (4)
T ln[(zf + A)/(z0 + A)]
By replacing and A in eq 4 by their respective expression
given in eq 3, the bubbling frequency of the cellulose fiber may
be rewritten as follows:
2RDc
f (5)
r(P + 2/r) ln[(zf + 10r)/(z0 + 10r)]
To go further with the dependence of the bubbling frequency
with both liquid and fiber parameters, we also can replace the
diffusion coefficient D0 in eq 5 by its theoretical expression
approached through the well-known Stokes-Einstein equation
(D0 kB/6d) with kB being the Boltzman constant (1.38
10-23 J/K) and d being the characteristic size of the CO2
molecules hydrodynamic radius (d 10-10 m).
In eq 5, by replacing each parameter by its theoretical
expression and each constant by its numerical value, the
variation of the bubbling frequency as a function of the various
pertinent parameters involved may be rewritten as follows (in
the MKSA system):
2[cL - kH(P + 2/r)]
f 2.4 10-14 (6)
r(P + 2/r) ln[(zf + 10r)/(z0 + 10r)]
The boundary layer thickness was indirectly approached
in a recent paper and found to be on the order of 20 m.8
Let us apply the latter equation to the standard textbook case
fiber displayed in Figure 1 and modeled in Figure 4 (i.e., r
5 m, z0 20 m and zf 100 m). Equation 6 may be
rewritten as the following by replacing the fibers parameters
r, z0, zf, and by their numerical values:
-8
2[cL - kH(P + 0.2)]
f 5.2 10 (7)
(P + 0.2)
In the latter expression, cL is expressed in g/L, kH is expressed
in g/L/atm, P is expressed in atm, and is expressed in kg/m/s
to fit the standards used in enology.
3.3. Relative Influence of Several Parameters on the
Average Bubbling Frequency. We will discuss the relative
influence of the following parameters on the average bubbling
frequency: (i) the concentration cL of CO2-dissolved molecules,
(ii) the liquid temperature , and (iii) the ambient pressure P.
(i) Through the use of eq 6 with every other parameter being
constant, the dependence of the theoretical average bubbling
frequency f with the CO2-dissolved concentration cL is in the
form f ) acL - b. By use of the high-speed video camera, a
few cellulose fibers that act as bubble nucleation sites on the
wall of a glass poured with champagne were followed with time
during the whole gas discharging process, which lasted several
hours. For each given nucleation site, the experimental bubbling
frequency fexp was directly accessed simply by measuring the
time Texp needed by the nucleation site to release a bubble
(therefore, fexp ) 1/Texp). The concentration cL of CO2-dissolved
molecules was indirectly accessed by using the growth rate of
bubbles just released from the nucleation site as a CO2-probe.
This method is developed in minute detail in ref 6 (see
Appendix). The dependence of the experimental bubbling
frequency fexp with cL is displayed in Figure 6 for four different
Kinetics of Bubble Nucleation in Champagne
Figure 6. Dependence of the experimental bubbling frequency fexp with
cL for four different bubble nucleation sites (at 20 C). Experimental
data show a linear-like dependence between fexp and cL, as expected
from the theoretical model displayed in eq 6.
nucleation sites. It is clear from Figure 6 that the dependence
of the experimental bubbling frequency follows a linear-like cL
dependence as was expected from the model developed in the
latter paragraph.
Furthermore, it is worth noting that the bubbling frequency
of a given nucleation site vanishes (i.e., the bubble release
ceases, f f 0 bubble/s), although the CO2-dissolved concentra-
tion remains higher than a critical value as demonstrated in a
previous paper.6 Actually, following both Laplaces law and
Henrys law, the curvature of the CO2 pocket trapped inside
the fibers lumen induces a concentration cB of CO2-dissolved
molecules on the order of kH(P0 + 2/r) in close vicinity of the
trapped CO2 pocket . Consequently, as soon as the concentration
of CO2-dissolved in the liquid bulk reaches a critical value c/L
) cB kH(P0 + 2/r), the diffusion toward the gas pocket
ceases and the given nucleation site stops releasing bubbles,
which is shown in Figure 6. Let us apply the latter condition to
the characteristic radius of a cellulose fiber6 (r 2 m). At 20
C, the critical concentration cL* in which below that bubble
release becomes impossible is
c/L kH(P0 + 2/r)
1.44 10-5(105 + 2 5 10-2/2 10-6) 2.2 g/L (8) tively. Increasing the liquid temperature by 10 K (let us say
In Figure 6, the wide range of different c/L displayed by
extrapolating the data to f ) 0 for each nucleation site followed
as time progresses is directly linked with the natural variability
of cellulose fibers that may be found in a glass of champagne
(in terms of lumens radius r). Actually, the typical range of
lumens radii may vary from about 1 to 5 m.5-8 By applying
eq 8, it is found that the typical range of c/L may vary from
about 1.7 g/L to about 2.9 g/L, which is clearly quite consistent
with the range of c/L found experimentally by extrapolating the
data to f ) 0 as shown in Figure 6.
(ii) The dependence of the bubbling frequency with the liquid
temperature is much more difficult to test experimentally in real
consuming conditions. Actually, we needed time to decrease
or increase the liquid temperature, and we found no satisfying
possibility of modifying the liquid temperature without signifi-
cantly losing CO2-dissolved molecules, which continuously
desorb from the supersaturated liquid matrix because of diffusion
through the liquid surface and because of bubbling from the
numerous nucleation sites found in the flute. We will discuss
J. Phys. Chem. B, Vol. 110, No. 42, 2006 21149
Figure 7. Theoretical dependence of the bubbling frequency f with
the temperature , as expected from the model displayed in eq 7, in
the range of usual champagne-tasting temperatures (from 5 to 15 C)
and for the textbook case fiber displayed in Figure 1.
Figure 8. Theoretical dependence of the bubbling frequency f with
the ambient pressure P (at 20 C), as expected from the model displayed
in eq 7 for the textbook case fiber displayed in Figure 1.
the theoretical influence of the liquid temperature by using eq
6. In eq 6, the temperature directly appears as 2, but the Henrys
law constant kH, as well as the dynamic viscosity , are strongly
temperature-dependent and expressed by eqs 1 and 2, respec-
from 278 to 288 K, which is approximately the range of
champagne-tasting temperatures) increases the theoretical bub-
bling frequency by about 50%. For the standard textbook case
fiber displayed in Figure 1 (r 5 m, z0 20 m, and zf
100 m) and with cL 10 g/L, the theoretical temperature
dependence of the bubbling frequency is displayed in Figure 7.
(iii) Increasing or decreasing the ambient pressure P also
significantly modifies the corresponding average bubbling
frequency f. For the standard textbook case fiber displayed in
Figure 1 (r 5 m, z0 20 m, and and zf 100 m) and
with cL 10 g/L, the theoretical pressure dependence of the
bubbling frequency is displayed in Figure 8. Reducing the
ambient pressure to only 0.3 atm (e.g., on the top of Mount
Everest) would increase the average bubbling frequency by a
factor of almost 3. This is basically the same phenomenon that
is responsible for gas embolism in divers who have breathed
high-pressure air under water when they resurface too quickly.
Inversely, if the ambient pressure is increased to 2 atm, this
decreases the average bubbling frequency by a factor of
about 2.
21150 J. Phys. Chem. B, Vol. 110, No. 42, 2006 Liger-Belair et al.

3.4. A Comparison with the Model by Uzel et al.9 The
model developed here is not the only one in the literature. The
one recently developed by Uzel et al. makes different assump-
tions about the way in which the bubbles form.9 Contrary to
the present model, which assumes that the dominant time scale
that controls bubble release is the growth of the gas pocket
growing trapped inside the fibers lumen, Uzels model es-
sentially assumes that the dominant mechanism is seeding at
the top of the fiber, the bubble detachment being controlled by
a balance between buoyancy and capillarity. Seeding at the
fibers tip necessarily involves unfavorable wetting conditions
of the fibers wall. Actually, because cellulose is a highly
hydrophilic material, aqueous liquids such as champagne and
carbonated beverages forbid the establishment of a triple contact
line at the fibers tip. Therefore, a gas bubble released after the
breaking of the gas pocket growing trapped inside the fibers
lumen (Figure 1, panel 5) should be unable to seed at the fibers
tip (as a droplet of water would do). However, some nucleation
sites could eventually experience transitions from wetting to
nonwetting conditions (due to lipid contamination, for example).
In such conditions, a bubble could definitely grow anchored to
the fibers tip before detaching because of buoyancy. In such
conditions, the total time needed to release a bubble from a
nucleation site would be the sum of two characteristic times:
(1) the time required by the gas pocket to grow from its initial
length, z0, to its final length, zf, as it reaches the fibers tip
(modeled in the present paper), and (2) the time required for
the bubble to grow until it detaches because of buoyancy
(modeled in the paper by Uzel et al.9). This is the reason why
these two extreme models are highly complementary. They focus
on both steps of the bubble release, the best model probably
being a combination of the two models. Mixing these two
models could be the purpose of future work.
4. Conclusions and Prospects
The dynamics of bubble nucleation from the lumen of
immersed cellulose fibers stuck on the wall of a glass poured
with champagne were accurately observed, in situ, from high-
speed video recordings. We used a previously developed model
that utilized the dynamics of the tiny gas pockets responsible
for the repetitive production of bubbles to access the theoretical
frequency of bubble release. The theoretical frequency of bubble
release was found to depend on various fiber and liquid
parameters. The main parameters likely to significantly influence
the frequency of bubble formation were found to be (i) the CO2-
dissolved concentration cL, (ii) the liquid temperature , and
(iii) the ambient pressure P.
In the future, we plan to organize at a large-scale champagne
terms of CO2 release, which we would like to both theoretically
and experimentally evaluate in the future.
Acknowledgment. The authors thank the EuropolAgro
institute and the Association Recherche Oenologie Champagne
Universite for financial support and Champagne Pommery and
Arc International for their collaborative efforts.
Appendix
The general equation concerning the mass transfer of
molecules from the bulk of a supersaturated liquid to a bubble
surface with time is
dN
) KAc (A1)
dt
where N is the number of transferred CO2 moles, K is the mass
transfer coefficient, A is the bubble area, and c ) cL - c0 is
the difference in CO2 concentration between the bulk of the
liquid and the bubble surface in equilibrium with the CO2 gas
into the bubble.
Assuming the gas into the rising bubble as ideal (PBV )
NR), the number of CO2 moles transferred into the bubble is
connected with the variation of its radius R with time as follows
dN PB dV PB dR
) ) A (A2)
dt R dt R dt
where V is the bubble volume, and PB is the pressure inside the
rising bubble assumed to be equal to the atmospheric pressure
P0, because both the hydrostatic pressure (FgH < 10-2P0) and
the Laplace pressure (2/R < 10-1P0) inside the rising bubble
are negligible.
By combining eqs A1 and A2, one obtains the rate of
expansion of the bubble radius
dR R
) Kc (A3)
dt P0
Generally speaking, heat and mass transfers are functions of
two dimensionless numbers, the Sherwood and Peclet numbers,
Sh ) 2KR/D0 and Pe ) 2RU/D0, respectively, with U being
the velocity of ascending bubbles. In the case of small and large
Pe, asymptotic solutions have been derived in the literature.
Most of them are listed in the book by Sherwood et al.15 During
ascent, champagne bubbles cover a range of high Pe between
approximately 102 and 105. At large Pe, Sh becomes proportional
to Pe1/3, with a numerical prefactor very close to unity.
Therefore,

( )
and sparkling wine tasting under a controlled atmosphere by KR 21/3 RU 1/3 U1/3
artificially modifying the intensity of effervescence through the w K 0.63D02/3 2/3 (A4)
D0 2 D0 R
ambient pressure parameter. We could eventually better under-
stand the role played by the intensity of effervescence on flavor Combining eqs A3 and A4 leads to
release without modifying the intrinsic aromatic properties of
the liquid (such as changes in the temperature would do). dR R U1/3
Actually, the continuous flow of ascending bubbles through the ) 0.63 D02/3 2/3 c (A5)
dt P0 R
liquid drains flavors and aromas with the result of continuously
renewing the layer at the liquid surface, thus providing a better By combining the empirical rising velocity U of ascending
release of the numerous volatile organic compounds above the champagne bubbles5 with eq A5, the rate of increase of the
liquid surface. However, bubbles bursting at the liquid surface ascending bubble radius becomes
also release a sudden and abundant quantity of CO2 above the
liquid surface with the result of irritating the nose during the dR R 2Fg 1/3
evaluation of aromas. From an enological point of view, there
k)
dt
0.63 D02/3
P0 9 ( )c (A6)
should therefore be a sort of ideal intensity of effervescence
that enhances flavor release without being too aggressive in where  is a numerical prefactor close to 0.7.
Kinetics of Bubble Nucleation in Champagne
Equation A6 was found to be in very good agreement with
the order of magnitude of experimental bubble growth rates in
champagne and beer glasses.5,6 Therefore, the good agreement
between experimental and theoretical bubble growth rates gave
us the idea to use the experimental rising bubble growth rate as
a probe for measuring c in the liquid medium. Finally, by
retrieving eq A6 in reverse order, c may be linked to the rising
bubble growth rate k and some liquid parameters as follows:
P0 9 1/3
c ) cL - c0
0.63R
D0-2/3 ( )
2Fg
k (A7)
where c0 ) kHP0 is the molar concentration of CO2-dissolved
molecules in equilibrium with the CO2 gas into the bubble.
Finally
P0 9 1/3
c L c0 + D -2/3
0.63R 0 ( )
2Fg
k (A8)
It is worth noting that in eq A8, each parameter is expressed
in the MKSA system. In particular, cL and c0 are expressed in
mol/m3.
Nomenclature
A ) bubble area, m2.
A ) variable depending on several parameters and has the
dimension of a velocity (see eq 3), m/s.
c0 ) molar concentration of CO2-dissolved molecules in
equilibrium (following Henrys law) with a partial pressure of
gaseous CO2 corresponding to the atmospheric pressure (i.e.,
c0 ) kHP0, mol/m3)
cB ) concentration of CO2-dissolved molecules around the
gas pocket in equilibrium with the pressure of CO2 molecules
in the vapor phase inside the gas pocket (following Henrys
law), mol/m3.
cL ) concentration of CO2-dissolved molecules in the bulk
of the supersaturated liquid medium, mol/m3.
c ) difference in CO2-dissolved concentrations between
the liquid bulk and the close vicinity of the bubble surface in
equilibrium with the gaseous CO2 into the gas pocket ) cL -
cB, mol/m3.
d ) characteristic size of the CO2 molecules hydrodynamic
radius (10-10 m).
D ) diffusion coefficient, m2/s.
D0 ) diffusion coefficient in the liquid bulk of CO2-dissolved
molecules, m2/s.
D ) transversal diffusion coefficient of CO2-dissolved
molecules inside the fiber wall, m2/s.
f ) frequency of bubble formation, bubbles/s.
fexp) frequency of bubble formation experimentally deter-
mined, in situ, from high-speed video recordings, bubbles/s.
kH ) Henrys law constant, kg m-3 ps-1.
k ) bubble growth rate dR/dt, m/s.
kB ) Boltzman constant, 1.38 10-23, J/K.
J. Phys. Chem. B, Vol. 110, No. 42, 2006 21151
K ) mass transfer coefficient, m/s.
N ) number of CO2 moles.
P ) ambient pressure, N/m2.
P0 ) atmospheric pressure, 105 N/m2.
PB ) pressure inside a bubble, N/m2.
Pe ) Peclet number, 2RU/D.
r ) radius of aperture of the lumen of a cellulose fiber acting
as a bubble nucleation site, 1-5 m.
R ) bubble radius, m.
R ) ideal gas constant, 8.31 J K-1 mol-1.
Sh ) Sherwood number, 2KR/D.
t ) time, s.
T ) period of bubble production, s.
Texp ) experimental period of bubble production, s.
U ) bubble velocity, m/s.
V ) bubble volume, m3.
z ) length of the gas pocket growing trapped inside a fibers
lumen.
z0 ) initial length of the gas pocket growing trapped inside
a fibers lumen.
zf ) final length of the gas pocket growing trapped inside a
fibers lumen, when it reaches a fibers tip.
Greek letters
 ) numerical prefactor in eq A6.
) thickness of the boundary layer, m.
) fluid dynamic viscosity, kg m-1 s-1.
F ) fluid density, kg/m3.
) liquid surface tension, N/m.
) temperature, K.
) characteristic time scale of the exponential-like bubble
growth (see eq 3), s.
References and Notes
(1) Liger-Belair, G. Uncorked: The Science of Champagne; Princeton
University Press: Princeton, NJ, 2004.
(2) Blander, M.; Katz, J. L. AIChE J. 1975, 21, 836.
(3) Lubetkin, S. D. Langmuir 2003, 19, 2575.
(4) Jones, S. F.; Evans, G. M.; Galvin, K. P. AdV. Colloid Interface
Sci. 1999, 80, 27.
(5) Liger-Belair, G. Ann. Phys. (Paris) 2002, 27, 1.
(6) Liger-Belair, G.; Vignes-Adler, M.; Voisin, C.; Robillard, B.;
Jeandet, P. Langmuir 2002, 18, 1294.
(7) Liger-Belair, G.; Topgaard, D.; Voisin, C.; Jeandet, P. Langmuir
2004, 20, 4132.
(8) Liger-Belair, G.; Voisin, C.; Jeandet, P. J. Phys. Chem. B 2005,
109, 14573.
(9) Uzel, S.; Chappell, M. A.; Payne, S. J. J. Phys. Chem. B 2006,
110, 7579.
(10) Liger-Belair, G.; Prost, E.; Parmentier, M.; Jeandet, P.; Nuzillard,
J.-M. J. Agric. Food Chem. 2003, 51, 7560.
(11) Autret, G.; Liger-Belair, G.; Nuzillard, J.-M.; Parmentier, M.;
Dubois de Montreynaud, A.; Jeandet, P.; Doan, B. T.; Beloeil, J.-C. Anal.
Chim. Acta 2005, 535, 73.
(12) Liger-Belair, G. J. Agric. Food Chem. 2005, 53, 2788.
(13) Liger-Belair, G.; Tufaile, A.; Robillard, B.; Jeandet, P.; Sartorelli,
J.-C. Phys. ReV. E 2005, 72, 037204.
(14) OSullivan, A. Cellulose 1997, 4, 173.
(15) Sherwood, T. K.; Pigford, R. L.; Wilke, C. R. Mass transfer;
Chemical Engineering Series; MacGraw-Hill: New York, 1975.