Journal of Food Engineering 50 (2001) 117120

www.elsevier.com/locate/jfoodeng

Research Note

Droplet size determination in food emulsions: comparison of

ultrasonic and light scattering methods
John N. Coupland *, D. Julian McClements
Department of Food Science, Food Colloids and Biopolymers Laboratory, University of Massachusetts, Amherst, MA 01003, USA
Received 26 November 1996; received in revised form 18 September 2000; accepted 4 November 2000

Abstract
Ultrasonic velocity and attenuation spectra (15 MHz) were measured for a series of corn-oil-in-water emulsions (20 wt% oil in 2
wt% polyoxyethylene sorbitan monolaurate) with a range of dierent mean droplet diameters (0.51.5 lm). Multiple scattering
theory was used to calculate mean diameters for each emulsion from both spectra. Droplet size was also determined using two
commercial light scattering instruments. All techniques showed the same general trend of decreased size with increased degree of
homogenization but there was only limited quantitative agreement between the various measurement techniques. 2001 Elsevier
Science Ltd. All rights reserved.
Keywords: Emulsion; Ultrasound; Particle-sizing; Light-scattering

1. Introduction
The colloidal properties of a food are important in
determining bulk qualities such as mouthfeel, appearance and rheology (Dickinson & McClements, 1995);
this is particularly true for food emulsions. A food
emulsion consists of a suspension of small oil droplets in
an aqueous continuum (e.g., milk, salad dressings, ice
cream mix) or vice versa (e.g., butter, margarine, chocolate). It is therefore important to develop methods to
accurately characterize the colloidal properties of food
emulsions.
The properties of a food emulsion that most contribute to its perceived characteristics are particle size
distribution and oil concentration. Direct determination of these parameters is dicult because droplets
are often too small to be resolved by conventional
light microscopy. Electron microscopy provides adequate resolution, but sample preparation is more disruptive and may generate artifacts. The most
commonly used technique for the characterization of
food emulsions is laser light scattering, but this is only
suitable for very dilute systems / < 0:05 wt% and

*
Corresponding author. Present address: Department of Food
Science, 103 Borland Laboratory, The Pennsylvania State University,
University Park, PA 16802, USA. Tel.: +1-814-865-2636; fax: +1-814863-6132.

dilution of more concentrated emulsions may disrupt

delicate aggregates. Nuclear magnetic resonance has
been used to characterize concentrated food emulsions
but the apparatus is expensive and dicult to operate
(Dickinson & McClements, 1995). Measurements of
the electrical properties of an emulsion can also be
related to its particle size distribution (e.g., Coulter
Counter, electroacoustic techniques), but these techniques are often limited to charged particles in a
conducting medium.
Techniques to extend the ease-of-use and versatility
of laser scattering particle sizing instruments to the more
concentrated emulsions commonly found in foods
would therefore be valuable. An ideal technique would
be reliable, rapid, and applicable to real food emulsions
under a range of process conditions. It would also be
advantageous to make on-line, non-invasive measurements for process control. Ultrasonic sensors have the
potential to meet many of these needs. It has been
shown that the scattering of ultrasound by an emulsion
is related to the size and concentration of the droplets as
well as the physicochemical properties of the component
phases (McClements, 1996). Various theories exist to
predict the ultrasonic properties of an emulsion (Allegra
& Hawley, 1971; Harker & Temple, 1988) as a function
of droplet size and concentration. By calculating the
particle size distribution that generates the best theoretical t to experimental measurements it is possible to
characterize an unknown emulsion.

0260-8774/01/$ - see front matter 2001 Elsevier Science Ltd. All rights reserved.
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J.N. Coupland, D.J. McClements / Journal of Food Engineering 50 (2001) 117120

2. Materials and methods

2.1. Materials
Polyoxyethylene sorbitan monolaurate (Tween 20)
was obtained from the Sigma Chemical Company (St.
Louis, MO). Corn oil was purchased from a local supermarket.
2.2. Sample preparation
Surfactant solution was prepared by dissolving 2 wt%
Tween 20 in distilled, deionized water. An emulsion was
prepared by homogenizing 20 wt% corn oil in surfactant
solution using a high speed blender (High Shear Homogenizing Container, Waring Laboratory, New Hartford, CT, 0.55 min), followed by sonication (Braun
Sonic-U, 060 s, maximum power) and high pressure
valve homogenization (Rannie 8.30R, Wilmington, MA,
0-3 passes, 1001000 bar). Samples were withdrawn at
dierent stages of the process to prepare a series of
emulsions of dierent size but similar composition. The
emulsions were coded 16 corresponding to increased
degrees of homogenization.
2.3. Light scattering
Two commercial static light scattering instruments
(Horiba LA-900, Horiba Instruments Incorporated, Irvine, CA and Malvern Mastersizer Model 3.01, Malvern
Instruments, Worcs., UK) were employed to measure
the droplet size distributions. A relative refractive index
of 1.08 (the ratio of the refractive index of the oil to that
of the surrounding aqueous phase) and an absorbance
index of 0.01 were used by the Horiba instrument to
calculate the droplet size distribution from the measured
light intensities; corresponding values were used by the
Malvern instrument (presentation code 0405). To prevent multiple scattering eects the emulsions were diluted with distilled water prior to analysis so the droplet
concentration was less than 0.02 wt%. All the emulsion
size distributions were approximately lognormal and
fairly monodisperse; representative examples
shown
P areP
in Fig. 1. The mean diameters (d32 ni di3 = ni di2 ,
where ni is the number of particles of diameter di ) are
reported in Fig. 3.
2.4. Ultrasonic measurements
The ultrasonic properties of the emulsions were
measured using a frequency scanning pulse echo reectometer (McClements & Fairley, 1992). All measurements were conducted at 19:0  0:1C using a pulsed (10
kHz) electrical spike signal (5900PR, Panametrics, MA),
and a 5 MHz broadband ultrasonic transducer (Panametrics, MA). No dilution was required in the ultrasonic

Fig. 1. Particle size distributions of representative emulsions determined by light scattering (Horiba LA-900). Emulsions 2, 4, and 6 (not
shown) had similar but slightly smaller distributions to those of 1, 3,
and 5, respectively.

method; samples were merely poured into the cell, allowed to thermally equilibrate (ca. 10 min) and measured (<1 s). Repeated measurements of the same
emulsion were very reproducible (velocity 0:1 m s 1 ,
attenuation 3%). Stirring the emulsions and repeating
the measurements on subsequent days caused no change
in the readings.

3. Results and discussion

Ultrasonic velocity (c; m s 1 ) and attenuation
(a; Npm 1 ) spectra were measured as a function of
frequency (f, MHz) for the emulsions (Fig. 2). Velocity
and attenuation both increased with frequency for all
emulsions.
The ultrasonic properties of 20 wt% monodisperse
corn-oil-in-water emulsions were calculated as a function of frequency, and diameter as described by
McClements and Coupland (1996) using physicochemical data was taken from the literature (Coupland &
McClements, 1998). The mean particle size was estimated from the ultrasonic spectra by iteratively adjusting
P the diameter, d, to minimize the function
cEXPTf j; where f is the frequency, and
f jcTHEORYf ;d
cEXPT and cTHEORY are the experimentally measured and
theoretically predicted velocity (or attenuation), respectively. The values from velocity and attenuation
sizing are shown alongside the light scattering measurements in Fig. 3. All particle sizing methods showed
the same expected trend, i.e., a larger degree of homogenization causing a decrease in size, however, there
was poor numerical agreement between methods,

J.N. Coupland, D.J. McClements / Journal of Food Engineering 50 (2001) 117120

119

Fig. 2. Ultrasonic velocity (a), and attenuation (b), spectra for corn-oil-in-water emulsions. Emulsions are numbered 16 (shown as j, , d, , N,
and M, respectively) with increasing degrees of processing.

Fig. 3. Mean droplet diameters determined by various methods.

Emulsions are numbered 16 with increasing degrees of processing.

particularly for large droplets. It is particularly surprising to see such poor agreement between the two
commercial light scattering instruments.
Adequate particle sizing depends on an ultrasonic
theory that completely describes the system under investigation. The theory used here works well at low
concentrations but above /  0:25 the quality of t
progressively declines as the multiple scattering eects
become more important (McClements, 1988). Although
the emulsions used here (/ 0:2) are within the established limits of the theory, it is possible that marginal
inaccuracy leads to imprecise sizing. The theory would
not be expected to perform well for occulated emulsions where multiple scattering eects would be very

important but as there was no change in the readings on

stirring the emulsions or repeating the measurements
over several days there is no evidence of emulsion instability in the present case. Another reason for poor
predictions from scattering theory would be inaccurate
physicochemical data used as constants in the calculations. The data used here (Coupland & McClements,
1998) were generated by averaging multiple data sets
from the literature but it is possible that the inherent
variability in samples is sucient to make them unreliable. Importantly, all of these reasons could be equally
applied to light scattering instruments with the important additional problems of sample disruption by dilution and the much more complex scattering theory used.
The ultrasonic particle sizing approach used here can
be used to generate a rapid mean diameter for an unknown emulsion, which would be valuable for process
control technologies (e.g., an automated control system
for a homogenizer). In other circumstances it may be
important to calculate a full size distribution by replacing d in the scattering theory with an appropriate
distribution function or the sum of several distribution
functions. The solution achieved here was based on a
single unknown, a full monodisperse distribution would
require at least two, a bimodal distribution ve, etc., and
it is expected that the additional precision of the t
would be unjustied from such a narrow region of the
spectrum.
In conclusion, it should be noted that a light scattering
instrument, whilst enjoying wide acceptance, does not
necessarily measure the true particle size. Ultrasonic
sizing is a new technique, but there is no reason the
measurements should be seen as less reliable. Indeed,
ultrasonic sensors may be more appropriate for the optically opaque, concentrated emulsions commonly found

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J.N. Coupland, D.J. McClements / Journal of Food Engineering 50 (2001) 117120

in foods. Commercial devices are already available to

measure the speed of sound in a liquid owing down a
pipe at a single frequency (e.g., Cygnus Instruments
Dorset, UK or GRC Instruments, Santa Barbara, CA),
which is typically related to solute concentration. Results
presented here suggest it would be possible to use these
sensors and a suitable calibration curve to estimate the
mean diameter of an emulsied food without the need for
additional hardware.
Acknowledgements
This material is based on the work supported by the
Cooperative State Research, Education, and Extension
Service, US Department of Agriculture, under Agreement No. 95-37500-2051. We are grateful to the laboratory of Prof. Stephanie Dungan for making some of
the light scattering measurements.

References
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suspensions and emulsions: theory and experiments. Journal of the
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Coupland, J. N., & McClements, D. J. (1998). Physical properties of
liquid edible oils. Journal of the American Oil Chemists Society, 74,
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Dickinson, E., & McClements, D. J. (1995). Advances in Food Colloids.
Glasgow: Blackie & Academic Professional.
Harker, A. H., & Temple, J. A. G. (1988). Velocity and attenuation of
ultrasound by emulsions. Journal of Physics D, 21, 3847.
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