Research: Science and Education
Zeroth Law, Entropy, Equilibrium, and All That
Sebastian G. Canagaratna
Department of Chemistry and Biochemistry, Ohio Northern University, Ada, OH 45810; s-canagaratna@onu.edu
Recently Gislason and Craig (1) discussed the question
of why two bodies in thermal contact come to a common tem-
perature. They also discussed problems involving systems not
in mechanical equilibrium. The discussion and the proofs given
by Gislason and Craig are, understandably, colored by their ap-
proach to thermodynamics (2–4). Gislason and Craig appear
to have eschewed the use of q, the quantity of heat transferred,
presumably because their approach does not favor it. They are
also critical of the traditional approach to solving such problems
and give the impression that these methods are lacking in rigor.
An examination of some popular physical chemistry texts as well
as some texts on thermodynamics revealed that discussions of
problems involving the establishment of pressure or temperature
equilibrium are difficult to find.
Most students would be more familiar with the tradi-
tional approach to thermodynamics than with the approach
of Gislason and Craig. It is therefore useful to re-examine the
problems discussed by Gislason and Craig using the methods of
traditional thermodynamics. In the traditional approaches the
use of q is not regarded as creating any problems. Using q, the
traditional approach treats the establishment of temperature or
pressure equilibrium without any loss of rigor. We also examine
how traditional thermodynamics would deal with entropy
maximization for some of the problems dealt with by Gislason
and Craig.
Gislason and Craig’s criticism of the traditional approach
to solving problems involving attainment of thermal equilib-
rium centers both on the concept of equilibrium as well as the
formulation and priority of the laws of thermodynamics in the
traditional approach. We therefore begin with a very brief review
of the salient aspects of equilibrium and the first and second
laws, together with a fuller treatment of the zeroth law. The three
laws enable us to examine whether the attainment of thermal
and mechanical equilibrium can be treated rigorously by the
application of the zeroth law, the law of mechanical equilibrium,
and the first law. We then discuss the role of the zeroth law in the
teaching of thermodynamics. Finally, some examples of entropy
maximization treated by Gislason and Craig are treated by the
traditional approach.
Equilibrium
Gislason and Craig state in the note of their article (1):
In thermodynamics, whenever the concept of equilibrium is
used prior to the development of the second law, this use is
provisional. The second law governs equilibrium: ...
They further state (ref 1, p 885) that it is the second law that
proves that thermal equilibrium does occur.
In the traditional approach, the concept of equilibrium
does not depend on the second law; the attainment of thermal
equilibrium is dealt with by the zeroth law, not the second law.
In fact, temperature is introduced first by the zeroth law, and it
732 Journal of Chemical Education  •  Vol. 85  No. 5  May 2008  •  www.JCE.DivCHED.org  •  © Division of Chemical Education
is then used in the formulation of the second law. It is important
to distinguish the concept of equilibrium from the conditions
that govern equilibrium. The concept of equilibrium itself only
requires that the independent variables of a system be constant
in time. For example, we find in Zemansky (5)
A state of a system in which Y and X have definite values
that remain constant so long as the external conditions are
unchanged is called an equilibrium state.
Here, Y and X are independent coordinates that describe the
system. To make this definite, suppose we define a sample of a
pure substance by its temperature T and pressure p, and these
were to remain constant in time. We would say that the system
is in equilibrium and we are invoking no particular law in using
the word equilibrium.
Three Types of Equilibrium
There are three aspects to the complete equilibrium of a
thermodynamic system (ref 5, p 26, and ref 6). These aspects
will be discussed in turn.
Mechanics recognizes an equilibrium referred to as me-
chanical equilibrium. This equilibrium is described in terms of
mechanical forces. For continuous systems, mechanical equi-
librium is described in terms of pressure. When such a system
is in mechanical equilibrium, the pressure of the system is the
same throughout. This condition for mechanical equilibrium is
referred to as Pascal’s law. If mechanical equilibrium does not
exist, a change will take place that will ultimately establish the
equality of pressures everywhere. Here we assume the absence
of surface, gravitational, electric, and magnetic effects. Thus the
law of mechanical equilibrium can predict, without invoking
the second law, the direction of change in the attainment of
mechanical equilibrium.
It is possible for a system to be in mechanical equilibrium
and still not be in complete equilibrium. Chemists are aware
that slow changes in chemical composition can take place
though the pressure and temperature are sensibly the same
everywhere. Chemical equilibrium is equilibrium with respect
to change of composition. It includes chemical reactions as
commonly understood, but in addition it includes phase changes
and diffusion due to differences in composition. The condition
for chemical equilibrium is governed by the second law of
thermodynamics.
A third type of equilibrium, thermal equilibrium, has to
be introduced because it was recognized that systems in me-
chanical and chemical equilibrium could still not be in equi-
librium when they are put in thermal contact. The importance
of the third type of equilibrium was the last to be recognized
though the consequences of this type of equilibrium had been
intuitively recognized earlier. The zeroth law was formulated
after the first and second laws of thermodynamics, but it was
considered to be more fundamental to the development of
 

traditional thermodynamics than the first and second laws of
thermodynamics and was therefore dubbed the “zeroth” law
of thermodynamics.
Complete (thermodynamic) equilibrium requires all
three types of equilibria. Mechanical and thermal equilibria
require the equality throughout the system of the pressure and
temperature, respectively. The second law deals with the condi-
tions for complete equilibrium. The condition for mechanical
equilibrium given by the second law is therefore exactly the same
as that given by Pascal’s law. Similarly, the condition for thermal
equilibrium given by the second law is exactly the same as that
given by the zeroth law. This should not be surprising, since there
clearly cannot be a conflict between different laws dealing with
the same subject. If we are interested only in thermal equilibrium
or in mechanical equilibrium, it is in general not necessary to
invoke the second law explicitly.
The First and Second Laws
The first law is applicable to both equilibrium and non-
equilibrium problems, but it does not govern the conditions of
equilibrium. In the traditional approach, the concept of work in
mechanics and the concept of adiabatic processes coming from
the zeroth law are used to introduce a property termed internal
energy, U. In some traditional approaches, the first law is used
to define a measure of the thermal interaction, called heat, q
(5–10). This approach is due to Born (11). Some authors prefer
to use a calorimetric definition of heat. The relationship between
the two approaches has been discussed recently (12). The con-
cept of work and heat in the Gislason and Craig approach differs
somewhat from the usual approach. A discussion of some aspects
of this approach has been given recently (13).
We will refer to the treatment in refs 5–9 as “traditional ap-
proaches”. Though there are slight differences in treatment, they
agree as to the values of heat and work to be assigned in any given
change. Most of the treatments found in the common physical
chemistry texts would be characterized as “traditional”.
The second law deals with the potential direction of change
and with the conditions for complete (thermodynamic) equilib-
rium. In the traditional approaches, the concept of temperature
(and therefore the zeroth law) is used to introduce an integrating
factor for q to define an extensive function termed entropy, S,
that (a) remains constant for an isolated system when the chang-
es in the isolated system are reversible and (b) increases when the
changes are irreversible. Subject to the conditions imposed on
the isolated system, the entropy is a maximum. The second law
also helps establish an absolute scale of temperature.
In addition to giving the conditions of equilibrium, the
second law may be used to make predictions about the stability
of the equilibrium state. The second law applied to the thermal
stability of systems shows that heat capacities must be positive
(ref 7, p 30).
The Zeroth Law of Thermodynamics
The content of the zeroth law is essentially this: there is a
property, which we shall call temperature, that governs a type
of equilibrium (to be called thermal equilibrium) that cannot
be explained in terms of mechanical forces. Thus the zeroth
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Research: Science and Education
law asserts that a complete description of a system must in
general include the specification of its temperature (or related
non-mechanical variable): we have moved from the domain of
mechanics to the domain of thermodynamics. The zeroth law
explicitly recognizes the concept of temperature and permits us
to establish an empirical temperature scale and thereby measure
temperature. Conventionally, the temperature scale is chosen
such that physiologically hotter bodies are associated with a
higher temperature.
Zemansky (ref 5, p 27) describes thermal equilibrium
thus:
Thermal equilibrium exists when there is no spontaneous
change in the coordinates of a system in mechanical and
chemical equilibrium when it is separated from its surround-
ings by a diathermic wall. In thermal equilibrium, all parts of
a system are at the same temperature, and this temperature
is the same as that of the surroundings. When these condi-
tions are not satisfied, a change of state will take place until
thermal equilibrium is reached.
Thermal equilibrium of a body implies a unique temperature
for it: every part of it has the same temperature. When we mea-
sure the temperature of a body we are using the principle that
temperature of the body is equal to that of the thermometer in
thermal contact with it. It would be illogical to suppose that
two bodies initially at temperatures T1 and T2 and placed in
thermal contact could be at two different temperatures when
they have reached thermal equilibrium, since the phrase thermal
equilibrium implies a unique temperature.
What can we infer about thermal interaction? We know
from experiment that the internal energy U of any body is an
increasing function of T. This implies that heat capacities, C,
are positive. Consider the thermal interaction of two samples
A and B of the same substance in an adiabatic enclosure but at
slightly different temperatures T1 and T2, with T1 > T2 Using
qA + qB = 0 and q = CdT it can be shown that the changes in
temperature are of opposite sign. Since A and B have a common
temperature at equilibrium, it follows that the hotter body gets
colder and the colder body gets hotter, and heat flows from the
hotter body to the colder body. Since the flow of heat depends
only on the temperature difference, we may take this as a general
result. Thus we are able to infer the direction in which heat flows
without appeal to the second law. Thus Callen (ref 14, p 39)
says, in reference to our intuitive notion of temperature: “we
should expect that heat should tend to flow from regions of high
temperature toward regions of low temperature”. Of course, the
second law will confirm this, but we know this result without
explicit appeal to it.
Is equilibrium necessary for measurement of temperature?
In their note Gislason and Craig (1) say
The zeroth law enables provisional thermometry and can be
stated as follows without using the concept of equilibrium.
When two systems (A and C) separately in good thermal
contact with a third system (B) cease to show changes in
measurable quantities, such as volume or resistance, the
two systems (A and C) have the same temperature. As a
consequence, the intermediary system (B) can be used as a
thermometer. ...
733
 Research: Science and Education
The words “cease to show changes in measurable quantities, such
as volume or resistance” are worth noting: in conjunction with
the idea of “good thermal contact” this is completely equivalent
to the concept of thermal equilibrium. Even though Gislason
and Craig are at pains to avoid mentioning the term thermal
equilibrium explicitly, the zeroth law cannot be stated without
at least implicitly using the ideas associated with thermal equilib-
rium. The measurement of temperature by a thermometer means
that both the thermometer and the body whose temperature
is being measured have the same unique temperature, and this
necessarily implies thermal equilibrium.
The Role of the Zeroth Law in Teaching
Students encounter problems involving two bodies initially
at different temperatures being placed in thermal contact early in
their physics course in high school. At this stage the emphasis is
on working intuitively, rather than being explicitly aware of what
laws are being used. There is a need for texts at a higher level to
re-work problems of this type with a more detailed explanation.
Most of the modern texts (5–10) in physical chemistry mention
explicitly the zeroth law. Even if no explicit mention is made of
the zeroth law, it is impossible to avoid using the consequences of
the zeroth law, since all that the law does is to put the concept of
temperature on a firm footing. Indeed, whenever we assume that
a body has a unique temperature, we have already used an impor-
tant result of the zeroth law. In solving problems, it is important
for students to know the general laws and principles governing
the phenomena being dealt with. The idea that there are three
aspects to equilibrium, viz., thermal, mechanical, and chemical, is
an important one and should be mentioned at the third-year col-
lege level. The result that all bodies in thermal equilibrium have a
common temperature and that this is the basis of thermometry
should also be discussed explicitly. Knowledge of these principles
will allow students to solve problems logically and appreciate the
relevance of the laws to problem solving.
Gislason and Craig claim (ref 1, p 885) that in the tradi-
tional method “the problem is solved by assuming that a single,
intermediate temperature is attained”. If the zeroth law has been
explicitly introduced, the above statement is not valid. Though
the first law does not require a unique final temperature, the
zeroth law does. The zeroth law assures us that there will be
a common temperature at equilibrium. Furthermore, it is not
necessary to assume that the final temperature lies between the
two initial temperatures. The final temperature comes out to
be the average of the two initial temperatures because we as-
sume that enthalpy, H, increases linearly with T and that both
objects have the same mass and specific heat capacities. It is dif-
ficult to see why the method should be characterized as “naïve”
(Webster: innocently direct but lacking in mental power!). The
traditional method seems brief, logically rigorous, direct, and
to the point.
Entropy Maximization in the Traditional Approach
According to the second law, spontaneous processes will
lead to an increase in the entropy of the universe. There is some
merit in verifying this, as Gislason and Craig have done, for
problems involving the establishment of thermal or mechanical
734 Journal of Chemical Education  •  Vol. 85  No. 5  May 2008  •  www.JCE.DivCHED.org  •  © Division of Chemical Education
equilibrium. We have to select, however, only examples where
this can be done without the mathematical details obscuring the
general principle.
The traditional approach uses dSsystem + dSsurroundings > 0 for
a spontaneous process. It is also customary for physical chemistry
texts to derive the fundamental equations (ref 10, p 105) such as
dH ≤ TdS + Vdp. But these equations are used in the texts only
for simple deductions such as dH ≤ 0 at constant entropy and
pressure. We will use these equations to explore the principle
of entropy maximization. It turns out that the same results
obtained by Gislason and Craig can be obtained more directly
and with much less mathematical manipulation.
It is possible to verify that the establishment of thermal
equilibrium under very general conditions leads to an increase
in the entropy of the universe. According to the zeroth law, two
bodies in thermal contact but at different temperatures are not
in thermal equilibrium. The second law asserts that the result-
ing flow of energy from the hotter body to the colder body will
always increase the entropy of the universe. We consider two
bodies A and B in thermal contact in an adiabatic enclosure. We
assume that A and B are in internal mechanical and chemical
equilibrium. Let B be at the higher temperature. We will, follow-
ing Guggenheim (7), use the symbol q to denote heat whether
it is finite or infinitesimal. Consider the flow of an infinitesimal
quantity of heat q from B to A. Then
q q
dSuniverse   (1)
TA TB
1 1
 q  > 0 (2)
TA TB
Thus, so long as the temperatures are different the entropy
of the universe continues to increase; when the temperatures are
equal dS = 0 and no further change will take place. This proves
that the entropy of the universe is a maximum. Note that apart
from the requirement of chemical and mechanical equilibrium,
we have not assumed any specific conditions for A and B, that is,
we have not required the pressure to be constant or the volume
to be constant and so forth. It follows that under all conditions,
when thermal equilibrium is attained the entropy of the universe
will be a maximum.
The above proof concentrates on the essentials. While the
examples considered by Gislason and Craig are good exercises in
“entropy analysis”, the above proof achieves, without distracting
details, the objective of verifying that the final state of thermal
equilibrium is a state of maximum entropy of the universe for
thermal interactions under all conditions.
In the Gislason and Craig approach to thermodynam-
ics, the proof of their eq 1 (as given in their appendix) is far
from trivial. In the traditional approach to thermodynamics,
if the bodies A and B are in an adiabatic enclosure at constant
pressure, then dUA+B = qA+B − pΔVA+B = ‒pΔVA+B so that
dHA+B = 0. Their eq 1 follows directly from this.
Appropriate fundamental equations may be used to
verify that the entropy is maximized in some of the specific
cases treated by Gislason and Craig. We first deduce very gen-
erally what conditions will lead to equilibrium. We then verify,
using the formula for the change in entropy, that if we start
 

with the final equilibrium state, any virtual change will result
in a decrease in entropy: the change in entropy is zero to the
first order in an infinitesimal parameter describing the change
(shows it is in equilibrium) and negative to the second order in
the same parameter (shows that the entropy is at a maximum).
The mathematical complexity is reduced because we are deal-
ing with infinitesimal changes. Our method may be regarded
as complementary to that of Gislason and Craig, since we start
with the final equilibrium state.
Constant Pressure, Equal Heat Capacities
Here we treat the case of two identical bodies A and
B interacting as constant pressure; this is the “classic case’’
treated by Gislason and Craig. The appropriate equation is
Research: Science and Education
confirms that the initial state corresponding to δ = 0 is a state of
maximum entropy.
General Constant-Pressure Problem
Here too we consider A and B in thermal contact at con-
stant pressure in an adiabatic enclosure, the temperature having
the unique equilibrium value, but the amounts and heat capaci-
ties of A and B being different. This introduces no new prob-
lems. When the enthalpy of A is increased by an infinitesimal
quantity ε and that of B is decreased by ε, then the magnitude of
the change in temperatures of A and B are ε∙CA and ε∙CB, where
CA and CB are the two heat capacities. We now have
the fundamental equation for dH. We assume that B has the dS tot  CA ln Tf  F /CA  C B ln Tf  F /C B (7)
higher initial temperature. From dH ≤ TdS + Vdp we get Tf Tf
dS ≥ (1∙T)dH − (V∙T)dp. Thus at constant pressure we get
TdS ≥ dH. Under the constraint dH = dHA + dHB = 0 the
F F
enthalpies of A and B will be such as to maximize the entropy.  CA ln 1   C B ln 1  (8)
Since dS = dSA + dSB, we have, at equilibrium CATf C B Tf

2 2
dH A dH B 1 1 1 F 1 F
dS    dH B  { CA  CB (9)
TA TB TB TA 2 CATf 2 C B Tf

For dS = 0 to be true for any change at equilibrium, the tempera-
tures TA and TB must be equal. As expected, the predictions of
the second law and the zeroth law agree. We now verify that the
entropy is at its maximum. We will do this by showing that for
the equilibrium state, any virtual change that alters the enthalpy
of A and B subject to the total change of enthalpy being constant
will decrease S. Let us increase HA by an infinitesimal quantity
and decrease HB by the same infinitesimal quantity. Since the
heat capacities are the same, the temperature of A will increase
to Tf + δ and the temperature of B will decrease toTf − δ: this
This confirms that the final state predicted by the zeroth law is
a state of maximum entropy. Note that we did not need to use
the value of the final temperature in the proof.
Variable-Pressure Problems
We now consider the variation of the volumes of the sub-
systems. Following Callen, (ref 14, p 43) we start with
1 p
defines the infinitesimal quantity δ. Using eq 2 of Gislason and dS s dU  dV (10)
Craig we see that the total change in entropy dStot from the T T
equilibrium state to the new virtual state is given by
which comes from the fundamental equation for U. If our sys-
tem is an isolated system consisting of two sub-systems 1 and
Tf  E T  E 2 in thermal contact, for all variations of U1 and U2 subject to
dS tot  Cp ln  Cp ln f (3)
Tf Tf dU1 + dU2 = 0 and for all variations of V1 and V2 subject to
dV1 + dV2 = 0, dS will be greater than 0 for non-equilibrium,
and equal to 0 for equilibrium. For any virtual process, since S is
E E already at its maximum, dS will be negative. We now have,
= Cp ln 1 + 1 − (4)
Tf Tf
1 1 p1 p
2 dS   dU 1   2 dV1 (11)
E T1 T2 T1 T2
 Cp ln 1  (5)
Tf
at equilibrium. Since U and V are independent variables, it fol-

2 lows that the coefficients of the two differentials on the right
E (6) hand side are separately equal to zero. This gives the result that
{ C
Cp
Tf both systems have the same temperature and pressure at equi-
librium. We could of course have obtained the same result from
This shows that any virtual change at equilibrium under the the zeroth law and Pascal’s law. The equilibrium value T of the
constraint of constant enthalpy leads to a decrease of entropy: temperature and the equilibrium value of the volume can be
the contemplated change cannot be a spontaneous change. This derived using the first law and the gas laws.

© Division of Chemical Education  •  www.JCE.DivCHED.org  •  Vol. 85  No. 5  May 2008  •  Journal of Chemical Education 735
 Research: Science and Education
To verify that this is a state of maximum entropy for the
case treated in Figure 1 of Gislason and Craig, we note that the
equilibrium values of V1 and V2 are both equal to V0∙2, where
V0 is the total volume. If we consider increasing the internal
energy of 1 and decreasing that of 2 by the same infinitesimal
quantity, the temperatures will increase and decrease by the same
infinitesimal quantity, say δ. Similarly, consider increasing V1
by an infinitesimal quantity ε from the equilibrium value and
decreasing V2 by the same quantity. For this change we have
one. For general problems involving spontaneous change, we
do not have any law other than the second law. The second law
not only deals with the direction of spontaneous change, but
also predicts that the entropy will be a maximum at equilib-
rium. We have seen that it is possible to know that heat flows
from the hotter body to the cooler body without explicit ap-
peal to the second law. Similarly, the laws of mechanics show
that if two gases at different pressures are brought together,
gas will flow from the higher pressure to the lower pressure.
Here too, the direction of change is obtained without explicit
T  E T  E appeal to the second law. The second law will, however, not
dS tot  n cV ln  n cV ln only predict this direction of change, but will also predict that
T T (12) the entropy will continue to increase during the change. This
V /2  F V /2  F principle of entropy maximization should certainly be grasped
 n R ln 0  nR ln 0
V0 / 2 V0 / 2
where cV is the molar heat capacity at constant volume, and n the
amount. Using the same manipulations as for the “classic case”,
we can show that all values of δ and ε bring about a decrease in
S, confirming that the system is already at its maximum.
How Best To Solve Problems
One of the stated aims of Gislason and Craig was to help
students gain confidence in the use of entropy to solve thermo-
dynamics problems. This, coupled with their poor opinion of the
use of the first law for solving problems involving spontaneous
change, suggests that they would be in favor of the use of entropy
in all problems of the type they have dealt with in their article.
They have also been critical of what they refer to as the “local
formulation” of the first law for the problems of interest in their
article. Are there any advantages in using entropy maximization
instead of the zeroth law, first law, and Pascal’s law?
Instructors will favor one path over another for the solu-
tion of a problem, depending on personal preferences as well
as the abilities of their students. However, it is reasonable to
require that instructors teach students always to proceed from
general principles. The fact that bodies in thermal equilibrium
have the same temperature is one such general principle. Often,
it is possible to use more than one set of general principles, one
set of general principles and laws being a subset of another.
It seems prudent in all cases to use the smallest subset that is
necessary to solve the problem. All the problems that Gislason
and Craig treated are capable of solution with the use of the
zeroth law, the first law, and Pascal’s law without loss of rigor.
Thus in the variable-pressure problem in their Figure 1, (ref 1,
p 887), the most direct approach, using the zeroth law, is that
U(1 mol, Ti, 2 atm) + U(1 mol, Ti, 1 atm) = U(1 mol, Tf, p) +
U(1 mol, Tf, p). Since the gas is ideal, and U depends on T only,
it is clear that Tf = Ti. Calculation of the pressure and volume is
now straightforward. The method given by Gislason and Craig
obtains the same result, but is considerably more complicated
because they use a larger set of general principles to begin with.
Even if we were interested in the change in entropy, the above
method would be shorter.
Favoring the use of the zeroth law, the first law, and Pas-
cal’s law for the sort of problems discussed here does not mean
that the principle of entropy maximization is not an important
736 Journal of Chemical Education  •  Vol. 85  No. 5  May 2008  •  www.JCE.DivCHED.org  •  © Division of Chemical Education
by students and verified in a few simple cases. The attainment
of both a unique temperature and a unique pressure gives the
condition of thermal and mechanical equilibrium. Problems
involving the attainment of only thermal and mechanical
equilibrium may be solved using these conditions supple-
mented by the first law and the necessary equations of state.
The second law comes into its own for chemical reactions.
For the problems dealt with here, the greater complexity of
the second law approach will militate against its adoption as
a general method of solution.
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