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There appears to be some confusion in the literature concerning the state of a granular mixture at the end of an
ideal mixing process, and this may have inuenced the basis on which some mixing indices were formulated. As an
attempt to provide clarication, we quantitatively established the three characteristic states of a granular mixture
the completely unmixed, the perfectly ordered, and the randomly mixed states by considering the relevant
probability distributions. We demonstrated how one may derive the expected values of various mixing indices based
on these probability distributions, and veried the results with a simple mixing simulation. Asymptotic arguments
showed the randomly mixed state, not the perfectly ordered state, best describes a well-mixed granular mixture,
while the two states become increasingly indistinguishable as the number of particles per sample increases. We
revealed that unlike the Lacey index, which is normalised based on the randomly mixed state, the normalisation of
the total entropy of mixing uses the perfectly ordered state, making it less than unity at the end of an ideal mixing
operation this has not been sufciently highlighted by the authors proposing such indices. We found it interesting
to analyse the Gini coefcient, a widely accepted measure of income inequality in economics, in the context of
granular mixing. While not advocating its use, we noted that similar to the other indices, its expected values for the
characteristic states are dependent on the choice of the basis of normalisation.
2014 The Institution of Chemical Engineers. Published by Elsevier B.V. All rights reserved.
Keywords: Granular mixing; Mixing index; Lacey index; Entropy of mixing; Gini coefcient
Corresponding author. Tel.: +64 226357788/99238137.
E-mail addresses: zgu231@aucklanduni.ac.nz (Z. Gu), j.chen@auckland.ac.nz (J.J.J. Chen).
http://dx.doi.org/10.1016/j.cherd.2014.04.014
0263-8762/ 2014 The Institution of Chemical Engineers. Published by Elsevier B.V. All rights reserved.
Please cite this article in press as: Gu, Z., Chen, J.J.J., A probabilistic analysis of some selected mixing indices. Chem. Eng. Res. Des. (2014),
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2 chemical engineering research and design x x x ( 2 0 1 4 ) xxxxxx
b number of cells
G Gini coefcient of income inequality in a popu-
lation; Gini coefcient of mixing for a granular
mixture 2. Characteristic states of a granular
H Shannon entropy of a probability distribution mixture
(nat)
M Lacey index 2.1. Representation and description of the
n number of particles in a random sample; characteristic states
number of outcomes in a discrete probability
distribution; number of individuals in a popu- The earliest discussion of the states of a granular mixture can
lation be attributed to Lacey (1943), where he illustrated the likely
N total number of particles in a mixture arrangements of particles at the end of an ideal mixing process
p probabilities in a discrete probability distribu- using schematics as shown in Fig. 1. Lacey argued that after
tion; fractions of a certain type of particles in a thorough mixing, Fig. 1(a) would correspond to what one may
cell hope to obtain, while Fig. 1(b) would be the best one is likely
P overall proportion of black particles in the mix- to achieve. Because these statements use vague expressions
ture such as hope to and likely, questions remain as to, rstly,
s2 variance of sample proportions how well the completely homogeneous state in Fig. 1(a) rep-
Si local entropy of mixing of cell i (nat) resents an actual well-mixed granular mixture, and secondly,
Stot total entropy of mixing (nat) whether it is of any importance to consciously differentiate
XCC cell count random variable between the two states in Fig. 1 when examining a granular
XSP sample proportion random variable mixture.
y income of an individual in a population (dol- We will address these questions by quantitatively estab-
lars) lishing the three characteristic states of a granular mixture. In
y average level of income in a population (dollars) order to facilitate visualisation, we shall represent particles in
a granular mixture as sites on a regular 2D rectangular lattice.
Greek symbols For simplicity, we will consider a binary mixture of black and
normalised Gini coefcient of mixing based white particles, so that each lattice site has a binary state for
on the perfectly ordered state colour for the particle at that site.
normalised Gini coefcient of mixing based There are various sampling methods for characterising
on the randomly mixed state the state of a given mixture. One common practice involves
tot normalised total entropy of mixing based on repeatedly taking random samples of a xed size and shape
the perfectly ordered state from the mixture with replacement, and recording the pro-
tot normalised total entropy of mixing based on portion of black particles within each sample; given that a
the randomly mixed state sufcient number of samples are taken, the distribution of
these sample proportions (denoted using the random variable
Subscripts XSP ) will characterise the state of the mixture. Alternatively,
0 expected value of the mixing index for the com- one can divide the entire domain of the mixture into a nite
pletely unmixed state number of xed cells, with the number of black particles in
p expected value of the mixing index for the per- each cell counted to give cell counts (denoted using the ran-
fectly ordered state dom variable XCC ); the state of the mixture can hence also
r expected value of the mixing index for the ran- be described by the distribution of these cell counts this
domly mixed state approach is particularly straightforward if the cells all con-
tain an equal number of particles. Other techniques, though
not considered in this work, include, for instance, counting
the contact points between different types of particles (Akao
of as ideal outcomes of mixing the implication is that the
et al., 1976).
resulting indices may be susceptible to incorrect interpreta-
In Sections 2.22.4, we will discuss the three character-
tion if one does not clearly understand the bases of their
istic states of a granular mixture and recapitulate existing
denitions. Therefore, we nd it important to differentiate the
understanding of these states in terms of the probability dis-
characteristic states of a granular mixture in quantitative and
tributions of sample proportions and cell counts.
probabilistic terms, and link such differences among the states
to the differences among the formulations of mixing indices
found in the literature.
It is also interesting to note that the concept of mixedness
has also been applied extensively in disciplines other than 2.2. The completely unmixed state
chemical engineering. Mixedness is frequently referred to by
alternative terminologies, such as species diversity in ecol- Prior to mixing, we normally expect the collection of particles
ogy (Lloyd et al., 1968), income inequality in economics (Sen, to be in a highly segregated state. Many possible congura-
1973), and racial segregation in sociology (Theil and Finizza, tions, such as those shown in Fig. 2, may be used to exemplify
1971), just to name a few. It is thus possible and of interest such a state, where particles of each colour cluster in a partic-
to adopt the mixedness concept in these other sciences and ular region of the lattice.
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Fig. 1 Pictorial representations of the likely arrangements of particles in a granular mixture at the end of an ideal mixing
operation used by Lacey (1943).
We may dene the completely unmixed state using the ide- which says that the sample proportion is always equal to the
alised case where a binary outcome can be associated with XSP , overall proportion of black particles in the mixture; that is to
which leads to a Bernoulli distribution for XSP , given by say, the outcome of random sampling is deterministic. We
can similarly expect the random variable for the cell counts
Pr(XSP = x) = Px (1 P)
1x
for x = 0, 1 (1) to follow
NP
where P is the overall proportion of black particles in the mix- Pr XCC = =1 (4)
b
ture. According to this distribution, any sample taken from the
mixture will either have a sample proportion of zero, when all As Thiel et al. (1981) have noted, the perfectly ordered state is
the particles in the sample are white, or unity, when all the only attainable in very special cases, and for the mixing of non-
particles in the sample are black, while the relative likelihood interacting particles that are only distinguishable by colour,
of either outcome is proportional to the overall proportion of
the respective type of particles.
By similar arguments, one can show that the distribution of
cell counts for a completely unmixed material should approx-
imately follow
N
Pr(XCC = x) = Pxb/N (1 P)
1xb/N
for x = 0, (2)
b
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the perfectly ordered state does not represent the nal state continuously measure sample proportions or cell counts and
of the mixture at the steady state. examine their distributions during mixing to track changes in
the mixedness of a granular material. It is often more conve-
2.4. The randomly mixed state nient, however, to adopt a certain numerical property of the
probability distributions as an effective measure of mixedness
Non-interacting particles that are identical except colour at rather than considering the specic distributions at all times.
the end of an ideal mixing operation will reach the randomly This leads to the creation of many of the mixing indices avail-
mixed state (Thiel et al., 1981). On a 2D lattice, this state is able in the literature: states of a granular mixture condense
represented by Figs. 4 and 1(b), the latter used by Lacey (1943). into probability distributions by the process of sampling, and
These randomly mixed states can be generated by completely the probability distributions further condense into mixing
randomising the arrangement of black and white particles on indices upon taking certain properties of the distributions.
the lattice, where the number of each type is set by a pre- Note how this process represents a cascade of information
scribed value of the overall proportion of black particles in the reduction, from the exact arrangement of particles in a gran-
mixture. ular mixture, eventually to the value of the mixing index.
Unlike the perfectly ordered state, random samples taken In this section, we will demonstrate the principle and the
from a granular mixture in the randomly mixed state will methods of forming measures of mixedness from appropriate
likely contain a different number of black particles each. Given probability distributions by considering both existing and new
a sample size of n, the distribution of sample proportions is mixing indices. The aim is to link our established understand-
approximated by ing of the states of a granular mixture to the expected values
and other distinctive features of various mixing indices.
n n(1x) 1 2
Pr(XSP = x) = Pnx (1 P) for x = 0, , , . . ., 1 (5)
nx n n
3.1. Simulation of mixing
a Prior to presenting our analysis of the different mixing indices,
where denotes a binomial coefcient. The mean and
b it is useful to consider how we might verify the results we are
variance of this distribution can be shown to be P and [P(1 about to derive for these indices. One way is to simulate a sim-
P)/n], respectively (Lacey, 1943, 1954). Note that the variance of ple granular mixing process and compute the mixing indices
the distribution of sample proportions for the randomly mixed as mixing takes place it is convenient to carry out such a
state asymptotically approaches zero in the limit of n : mixing process directly on the lattice that we have been using
this implies that the two states become increasingly indistin- throughout this paper for the illustration of ideas. As to how
guishable as the number of particles per sample increases. we will induce mixing on the lattice, note that we are not too
However, for a granular material, unlike a uid, there are only concerned with the mixing method, namely, the set of rules by
a nite number of particles in any sample taken; thus, the per- which the mixture gets mixed progressively. This is because
fectly ordered state and the randomly mixed state are indeed the characteristic states of primary interest are all close to the
two dissimilar states. beginning or the end of the mixing operation, largely inde-
Finally, the probability mass function of XCC for the ran- pendent of the path of changes that the mixture follows. Thus,
domly mixed state can be written as we simply need a random process that continuously increases
the mixedness of particles on the lattice many methods are
N/b N/bx N possible (e.g., Too et al., 1979), but we will hereinafter limit
Pr(XCC = x) = Px (1 P) for x = 0, 1, 2, . . ., (6)
x b ourselves to one method that is adequate for the purpose of
generating the mixing data.
whose mean and variance are (NP/b) and [NP(1 P)/b], respec- Black and white particles were initially arranged on a 100-
tively. by-100 square lattice as shown in Fig. 5(a), representing an
instance of the completely unmixed state this state corre-
3. Measures of mixedness sponded to step 1 of the mixing process. The overall proportion
of black particles was chosen to be P = 0.25. An algorithm was
We have demonstrated how probability distributions can be then applied recursively to the lattice to cause mixing in dis-
used to characterise states of a granular mixture with differ- crete steps, each of which corresponded to a number of similar
ent degrees of mixedness; using such relationships, one may actions, where a single action randomised the distribution of
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Fig. 5 Arrangement of particles at selected steps from the simulated mixing process.
particles inside a 4-by-4 square region. A single step of mix- probability distributions. For the completely unmixed state,
ing then required this mixing action to be repeated until the the distribution of sample proportions, XSP , is given by Eq. (1);
region had assumed all 952 possible locations it can occupy thus, the expected value of the variance of sample proportions
in the mixture exactly once, following a random sequence of for the completely unmixed state is
these locations. A total of 300 of these steps of mixing were
performed. Fig. 5 shows the arrangement of particles on the 2 2
s20 = E(XSP
2
) [E(XSP )] = (0 + P) (0 + P) = P(1 P) (7)
lattice at selected steps.
Several mixing indices were calculated at every step of
The distribution XSP for the randomly mixed state is given by
mixing from the distributions of sample proportions and cell
Eq. (5); we have noted that the variance of this distribution is
counts. This requires either obtaining random samples from
equal to
the mixture or dividing the domain into cells. A total of 5000
square samples, 5-by-5 in size (hence n = 25), were taken at
P(1 P)
random locations within the mixture at every step, with the s2r = (8)
n
proportions of black particles in the samples noted; mean-
while, the domain was also divided into 400 xed square cells Eqs. (7) and (8) simply reproduced the results of Lacey (1954).
(as indicated by the regions enclosed by the lines in Fig. 5(g)), For the perfectly ordered state as described by Eq. (3), the vari-
also 5-by-5 in size, with the count of black particles in the cells ance of sample proportions for the perfectly ordered state is
noted. The results of the calculated mixing indices are to be given by the trivial result
presented in Sections 3.23.4.
It should be noted that when one takes random samples, s2p = 0 (9)
the mixing indices calculated for even the same state of the
mixture would involve variability as a result of sampling. Since
We will now consider the well-known Lacey index (Lacey,
our work focuses on the expected values of the mixing indices,
1954), dened as
as many as 5000 random samples were taken at every step
of mixing to calculate the mixing indices, in order to min-
s20 s2
imise any statistical noise due to sampling. Taking such a large M= (10)
number of samples is rarely feasible in practice, so it would s20 s2r
be plausible to appeal to statistical inference in practical sit-
uations when one calculates mixing indices from a limited Since s20 and s2r are xed with given P and n, it is useful to think
number of samples. of the Lacey index as a normalised version of the variance
of sample proportion. Because the normalisation is based on
the completely unmixed and the randomly mixed states, the
3.2. Variance of sample proportions; the Lacey index expected values of the Lacey index for these two states are
M0 = 0 and Mr = 1, respectively. As the mixture evolves from
A large portion of the mixing indices available, especially those the completely unmixed state to the randomly mixed state
found in the early literature (e.g., Lacey, 1943, 1954; Beaudry, during a typical mixing process, the variance correspondingly
1948; Blumberg and Maritz, 1953), are based on or related to decreases from s20 and converges to s2r , while the Lacey index
the variance of sample proportions, commonly denoted as s2 . increases from zero to unity.
The expected values of the variance of sample proportions It is important to note that the above process does not
for the characteristic states can be derived from appropriate involve the perfectly ordered state. The expected value of the
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1
b
We will rst state the mathematical denition of the Shan-
Stot = Si (14)
non entropy in information theory (Shannon, 1948): consider a b
i=1
discrete probability distribution with n outcomes, correspond-
ing to the events E1 , . . ., En with probabilities p1 , . . ., pn ; given
It is apparent from Eq. (13) that, for a binary mixture, the
exactly one of the n events is bound to occur, the Shannon
local entropy is simply a function of the fraction of black parti-
entropy of the distribution, H, is dened as
cles in the cell. This functional relationship is shown in Fig. 7,
and is a frequently quoted result in information theory. We
n
H= pi ln pi (12) observe that the local entropy is maximised when pi = 0.5 in
i=1 a cell, which corresponds to a local entropy of ln 2.
As was done for the variance, we will derive the expected
When the natural logarithm is used in the denition in Eq. (12), values of the total entropy for the characteristic states. For the
the Shannon entropy has the unit nat. The Shannon entropy completely unmixed state, the distribution of cell counts, XCC ,
has a number of interesting properties and can be interpreted given by Eq. (2), suggests that the fraction of black particles in
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1
n n
where XCC,i and XCC,j are independent random variables hav-
G= yi yj
(20) ing a probability distribution identical to XCC . Note we can also
2n2 y
i=1 j=1 calculate the Gini coefcient of mixing using the Lorenz curve,
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Gp = 0 (22)
G0 = 1 P (23)
For the randomly mixed state, we will approximate XCC using Fig. 12 The Gini coefcient of mixing from the simulated
a normal distribution where the mean and variance are iden- mixing process.
tical to those of the binomial distribution given by Eq. (6), i.e.,
XCC N(NP/b, NP(1 P)/b). Subsequently, we can derive (Gu and
Chen, 2013) the expected value of the Gini coefcient of mixing
for the randomly mixed state, yielding
b(1 P) In a typical granular mixing process where the binary mix-
Gr = (24)
NP ture changes state from completely unmixed to a randomly
mixed, the Gini coefcient of mixing will start from G0 , which
To summarise, approximate values of the Gini coefcient of is always below unity, and approach Gr , which is always above
mixing for the characteristic mixtures can be determined from zero, as long as the number of particles per cell is nite. For the
the analytical expressions given by Eqs. (22), (23), and (24). simulated mixing process, the changes in the Gini coefcient
Once again, note that as (N/b) , Gr Gp , implying that are shown in Fig. 12. Akin to how the normalised total entropy
the randomly mixed state asymptotically converges to the of mixing does not converge to unity at the steady state of mix-
perfectly ordered state in the limit of very large cells. ing, the Gini coefcient of mixing similarly does not converge
We will now consider the problem of normalisation of the to zero as such is its expected value for the perfectly ordered
Gini coefcient as we did for the previous indices. Interest- state.
ingly, the Gini coefcient is a naturally normalised index and One may make an attempt at normalising the Gini coef-
is bounded below and above by zero and unity as entailed by cient with different bases so that it behaves more similarly
its denition we have noted this fact when discussing the to the established mixing indices like the normalised total
Lorenz curve earlier in this section. entropy, whose value starts at zero for the completely
a
The values of Stot,r and Stot,p can be evaluated from Eqs. (17) and (16), respectively.
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unmixed state and increases with a higher degree of mixed- of the characteristic states used for the normalisation indices
ness. A possible normalisation of such kind is given by such as the Lacey index (M) are normalised based on the ran-
domly mixed state, while indices like the normalised total
G0 G G0 G G entropy of mixing (tot ) are normalised based on the per-
= = =1 (25)
G0 Gp G0 0 G0 fectly ordered state. As a granular mixture tends towards the
randomly mixed state as the equilibrium mixture of an ideal
which is analogous to the normalisation of the total entropy
mixing process is achieved, the Lacey index will approach
of mixing in Eq. (18). Another possible normalisation is
unity while the normalised total entropy will stabilise at a
G0 G value below unity. Being aware of such features of the mix-
= (26) ing indices when one uses them is an essential prerequisite
G0 Gr
for correctly interpreting them.
which makes the normalisation akin to that used for the Lacey We have examined the Gini coefcient from the study of
index found in Eq. (10). One can choose from either of the income inequality in economics, dened the Gini coefcient
two normalised indices as long as the consequences that arise of mixing for granular materials, and highlighted its properties
from the normalisation used are noted. as a possible mixing index.
A key achievement from our analysis of the Gini coef-
cient of mixing is that we have illustrated how the formulation
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Please cite this article in press as: Gu, Z., Chen, J.J.J., A probabilistic analysis of some selected mixing indices. Chem. Eng. Res. Des. (2014),
http://dx.doi.org/10.1016/j.cherd.2014.04.014