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Journal of Electroanalytical Chemistry 482 (2000) 110 116

QED coherence and electrolyte solutions

E. Del Giudice a, G. Preparata a,*, M. Fleischmann b
a

Department of Physics and INFN, Uni6ersity of Milan, Via Celoria 16, 20133 Milan, Italy
b
Bury Lodge, Duck Street, Tisbury, Salisbury, Wilts SP3 6LJ, UK

Received 8 July 1998; received in revised form 23 December 1999; accepted 7 January 2000

Abstract
In the framework of quantum electrodynamics (QED), the universally accepted theory of ordinary condensed matter, we
analyse a system of ions dissolved in water. Contrary to the common opinion that for aqueous solutions in normal conditions,
QED can be well approximated by classical physics or by the semiclassical approximations of molecular dynamics, we find for
such systems QED solutions of a very different nature. Such solutions appear to solve several paradoxes that plague the
conventional approaches. Our main result is that ions dissolved in water are not in a gaseous state, but settle in a coherent
configuration, where they perform plasma oscillations in resonance with a coherent electromagnetic field, thus providing a
satisfactory understanding of the thermodynamics of electrolytes. In this new framework, we also find a simple explanation of the
phenomenon of osmosis. 2000 Elsevier Science S.A. All rights reserved.
Keywords: Quantum electrodynamics; Electrolyte

1. Introduction
The answer has now been sought for nearly two
centuries to the following simple question: what is the
nature of the virtue (or 6is as our forefathers used to
call it) of water and other polar liquids which compensates for the high stability of ionic lattices so as to
produce electrolyte solutions?
We observe that the lattice energy and dynamics of
such solids are interpreted presently in terms of the
generally accepted electrostatic picture of matter. The
formation of strong electrolytes has then been attributed (since the time of Arrhenius [1]) to the ionic
character of the salts themselves coupled to the high
dielectric constant, e.g. of water (e =80 at 300 K). It is
assumed that the Coulombic forces in the lattice are
reduced by a factor e thereby allowing a separation of
the ions with only negligible changes of enthalpy (e.g.
see Nernst and Thomson [2 4]). However, the dielectric
constant is a purely phenomenological observable describing the bulk properties of the medium. While it is
certainly true that two charges separated by se6eral
* Corresponding author.
E-mail address: preparata@mi.infn.it (G. Preparata)

layers of water will interact with a force e times smaller

than in vacuo the NernstThomson argument has to
circumvent the difficulty that the ionic lattice is not
immersed in water but in a vacuum. We then need to
explain the way in which we can surmount an energy
barrier of the order of 5 eV in order to insert a single
layer of water (thickness: 3.2 A, ) between the ions.
We need to ask: what physically reasonable interaction is there in water to offset such large energy imbalances? Modern molecular dynamists might be tempted
(and, indeed, have been) to invent all manner of twobody potentials between the water molecules and ions
to explain such phenomena. However, such explanations are physically unmotivated for they rely on a
panoply of two- and three-body potentials, whose common feature is a large electric polarisability of the water
molecule in the ground state. We maintain, instead,
that such a crucial feature is totally baseless for the
following reason: second order perturbation theory ties
the polarisability of H2O in the ground state to its
spectrum and to the transition probabilities (oscillator
strengths) between the ground state and the excited
states. A rapid survey of both kinds of experimental
information shows that the hardness of the spectrum
(the first excited state being at 7.6 eV) and the smallness

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E. Del Giudice et al. / Journal of Electroanalytical Chemistry 482 (2000) 110116

of the oscillator strengths [5], make the H2O molecule a

very stiff object, totally at variance with the polarisability required by the potentials used in molecular dynamics. Thus the only electrostatic interactions that H2O in
the ground state is capable of exerting are related to its
rather modest electric dipole (corresponding to two unit
charges separated by 0.38 A, ), which thus cannot compensate the attractive force between two opposite
charges at the same distance.
We have to conclude that the Coulombic attraction
can be damped out by the dielectric constant of water
only after an energy barrier of approximately 5 eV has
been surmounted, a phenomenon which cannot be explained by electrostatics. In this paper we shall show
how the basic question can be answered in a natural
and simple manner by adopting the concepts of QED
[6].

2. The short-time dissociation process

As a first step in the overall process

A+B
lattice Asolution + Bsolution

(1)

we consider the highly endothermic transition to neutral species

A+B
lattice +H2O A +H2O +B

(2)

whose energy deficit D(AB A + B) can be obtained

from standard thermodynamic data (Table 1). In view
of the large value of D(AB A + B) (: 6 eV for most
strong electrolytes) such transitions can be only virtual
and, consequently, can last only for the time given by
the Heisenberg principle unless there is a further transition from such a virtual configuration to another which
compensates the energy gain D(AB A + B). Before
showing how this can be achieved, we note that the
system can undergo the transition to the ionic
configuration
+

A +H2O + BA + H2O +B

(3)

with the expenditure of a rather small energy given

approximately by
D(ABA+ + B): 1/e(E(A+)+ E(B))

where E(A+) and E(B) are the ionisation energy of A

and electron affinity of B in vacuo, e is the dielectric
constant of water which, as we shall see below, is given
by the simple Frohlich value
einc = 1+

H
H
Na
Na
K
K
Li
Li

OH
Cl
Cl
OH
OH
Cl
OH
Cl



d 2w N
3T V

(5)

where dw = 0.38 A, , e is the static dipole of water and

(N/V)w is its density1. At 300 K, einc : 12 which is
much smaller than the bulk value. The simple result
(Eq. (4)) can be understood if we consider that due to
the strong dipole field of the water molecule, the electron bound inside A becomes free and is attracted by
the electron affinity of B. The energy balance of this
electron transfer which would be given by E(A+ +B)
in vacuo is now damped by einc which applies to the
parts of the system where dissolution takes place.
We observe that it is a consequence of QED coherence [6], that water forms two interpenetrating fluids
[7], one made up of an array of coherence domains
(CDs) in which the water molecules oscillate in phase
with a condensed, coherent classical e.m. field, the other
consisting of a dense vapour of incoherent molecules
formed by evaporation from the CDs due to thermal
fluctuations. Due to the basically ordered state of the
molecules in the CDs (the hydrogen bonded network),
the AB molecules can dissolve only in the incoherent
phase (see below) whose dielectric constant is given by
the simple Langevin theory (Eq. (5)). Needless to say,
the much larger ebulk is given to a first approximation
by the combination
ebulk =

Ncoh
N
ecoh + inc einc
N
N

(6)

where Ncoh/N and Ninc/N are the coherent and incoherent fractions, respectively2.

DE/eV

DE/eV

D(AB A+B)

D(AB A++B)

5.63
4.48
6.65
5.94
5.75
6.73
7.10
7.17

+0.58
0.78
+0.04
0.46
0.60
+0.18

0.38

dDE

The short time dynamics of the dissociation process

leads us to the conclusion that a salt can dissolve to

H2O
HCl
NaCl
NaOH
KOH
KCl
LiOH
LiCl

(4)

3. The DebyeHuckel coherent plasmas

Table 1
Data obtained form Ref. [12]
AB

111

5.05
5.26
6.61
6.40
6.35
6.55

6.78

In Eq. (5) and throughout this paper, the natural unit system is
used, where ' (Plancks constant)= c (speed of light)= kB (Boltzmanns constant)=1; the only dimensional unit is a length. For
instance, 1 eV = 5 104 cm 1, 1 K=4.31 cm 1, 1 Debye=6.23
10 10 cm, e =0.3 (adimensional).
2
From the calculated fractions [6], we estimate ecoh =160, a very
high value which gives important information about the structure of
the coherent fluid. We will return to this aspect in a future publication.

E. Del Giudice et al. / Journal of Electroanalytical Chemistry 482 (2000) 110116

112

form an electrolyte solution only, provided the ions A+

and B, once separated by a layer of water molecules,
undergo a dynamical process which provides an energy
loss comparable to the large barrier D(AB A + B). If
this is not the case, then energy conservation would
require that the ions should fall back to their initial,
stable, configuration. This is the basic reason why the
formation of electrolyte solutions is excluded by a
purely electrostatic model of the interactions in condensed matter. We will show in this section how QED
provides the missing factor by virtue of the coherent
collective interactions between the ions.
We use the Debye Huckel theory [8,9] as the starting
point of our discussion and, according to our theory of
water [7], locate the ions in the coherent fraction where
the effective dielectric constant einc :12 (T =300 K)
(the structure of the incoherent fraction such as would
arise from the hydrogen bonded network will exclude
the electrolyte)3. The conventional Debye Huckel theory predicts a charge density distribution around a
positive ion placed at the origin of a three-dimensional
co-ordinate system:
r(r) =



where
k2=

ek 2 exp(ka) exp( kr)

,
4p 1+ka
r

2e 2 N
eT V

(r \a)

rCI =

(8)

(12)

where the plasma frequency vP is given by

vP =



e N
V
m 1/2
I

1/2

(13)

The condition (Eq. (12)) takes the form

g 2 = 0.93c 1/2 ] 0.59

(14)

which is therefore satisfied for c5 15. For sufficiently

large values of g, we derive the energy loss per ion [6]
E
4p v 2P 2
DI = =2vIa 2maxg 2 =
a
N
3 vI max

(15)

where a 2max, the maximum amplitude of the oscillation

of the ions is given by
4
mv
k2 I I

(16)

Combining the various quantities, we obtain the truly

remarkable result
DI =

8p
eT
3

(17)

i.e. a gap that is dependent only on the temperature and

on the dielectric constant (which is itself temperature
dependent). Thus due to the superradiant plasma oscillations, the pair of ions gain the energy
DA+B = DA+ + DB =

16p
eT
3

(18)

rr(r)r dr
=
r(r)r 2dr

2
k

3k 3
3
=
r =
3
4prCI 32p

(9)

(10)

The plasma frequency of the A+ ions is then given by

 

2p vP
16
]
3 vI
27

a 2max = mIvIr2 #

and evaluating the mean charge density of these counter ions as

vA+ =

g2=

(7)

a is the radius of the ion and (N/V) is the ionic

concentration. The form of Eq. (7) shows that the
plasma is far from ideal (where ideality requires a
constant density of the neutralising fluid). We note also
that such plasma must undergo oscillations whose frequency can be estimated by determining the mean
radius rCI of the charge distribution of the counter
ions

&
&

where mA is the mass of the A+ ion. A similar formula

with mA replaced by mB holds for vB4.
We can now ascertain whether the plasmas of ions
access a strongly coherent state, thereby developing an
energy gain. From the theory of non-ideal plasmas [6],
the required condition is that the coupling constant

 

e
3k 3
1/2
e m A 32p
1/2

which at 300 K amounts to about 5.2 eV!

4. Discussion and conclusions

We need to consider first of all the qualitative differences between the conventional DebyeHuckel theory
and the model which we have outlined in the previous
sections. In the conventional theory, the interaction

1/2

(11)

This hydrogen bonded network has a different origin from that

normally considered and also has a different structure [10]. The water
molecules spend about 13% of their time in the 5d state of H2O. This
state fills the interstices between neighbouring molecules and thereby
excludes other species from the coherence domains.

4
The value of this frequency at 300 K is: vI =1.56 103(mP/mI)1/
2c 3/4 cm 1, or nI =7.4 103(mP/mI)1/2c 3/4 GHz, where c is the molar
concentration of the solution. Note that, according to the theory of
coherent QED interactions, the ions in the incoherent fraction of the
water in turn create a coherence domain whose size is given by
lI =2p/vI, i.e. about 40 mm for m = mP and c =1.
5
For c ]1 one can infer from the condition rCI =2.44 10 8
c 1/2 cm that the theory must take a more elaborate form.

E. Del Giudice et al. / Journal of Electroanalytical Chemistry 482 (2000) 110116

113

Table 2
Ion kept fixed

(AB)(AB)%

D(I)D(I%)

Exp/eV

Naive theory equation

(Eq. (4)) (1/e)(E(I)E(I%))/eV

H+
Na+
K+
OH
Cl
OH
Cl
Cl
OH
Cl
Cl
Cl

H2OHCl
NaOHNaCl
KOHKCl
H2ONaOH
HClNaCl
H2OKOH
HClKCl
HClLiCl
NaOHKOH
NaClKCl
NaClLiCl
LiClKCl

D(OH)D(Cl)
D(OH)D(Cl)
D(OH)D(Cl)
D(H+)D(Na+)
D(H+)D(Na+)
D(H+)D(K+)
D(H+)D(K+)
D(H+)D(Li+)
D(Na+)D(K+)
D(Na+)D(K+)
D(Na+)D(Li+)
D(Li+)D(K+)

0.21
0.21
0.20
1.34
1.34
1.29
1.28
1.51
0.05
0.06
0.17
0.23

0.15
0.15
0.15
0.7
0.7
0.77
0.77
0.68
0.07
0.07
0.02
0.09

between the ions in solution is discussed in the framework of classical electrostatics and such a formulation
gives a well-defined variation of the interaction energy
(the minor term) with the concentration. The critically
important question of why lattices should dissolve in
the first place is not considered per se but, instead, is
dealt with separately by using the macroscopically observed dielectric constant to explain the reduction of
the ionic interaction energy within the lattice (the major
term).
Such arguments are clearly incomplete because the
ions in solution do not form a static ensemble (except
at absolute zero!). If we use instead electrodynamics, we
find that the solvent (water) itself divides into coherent
and incoherent domains [6]. The coherent domains will
exclude the ionic components which will therefore be
confined to the incoherent fraction. The electrolyte in
this fraction will in turn form coherence domains.
If we turn to more quantitative aspects, we see that
the success of the Debye Huckel theory requires that
the major term be rigorously constant, so that the ionic
interaction energy is given by the minor term alone.
The reason why this should be so has never been
discussed. On the other hand, the electrodynamic theory gives an immediate explanation (Eq. (18)) provided
the ions are confined to the incoherent fraction of the
solvent. Moreover, this theory explains why the salts
dissolve in the first place and gives an estimate of the
solvation energies without involving the macroscopically observed dielectric constant.
We consider next some quantitative aspects of the
theory which we have outlined in this paper. Table 1
gives the experimental values of the dissociation energies DE(AB A +B)vacuum, DE(AB A+ +B)water,
together with their differences
dDEAB = DE(AB A +B)vacuum
+DE(AB A+ +B)water

(19)

for a number of binary electrolytes. The large values of

dDE show that a purely electrostatic picture does not

provide a dynamical mechanism for surmounting energy barriers as high as dDE.
On the other hand, we have shown in the last section
that the coherent electrodynamic oscillations of the
DebyeHuckel plasmas lead to an energy term (Eq.
(17)) which is about 2.6 eV per ion. We can therefore
now check whether the dDE values calculated in Table
1 agree with our theory, which predicts
dDEAB =

16p
eT+ D(A+)+ D(B+)
3

=[D(A+) D(A+%)]+ [DB+) D(B+%)]

(20)

whereas a simple electrostatic calculation would give

1
D(I)= E(I)
e

(21)

where E(I) is the ionisation energy or electron affinity

of the corresponding ion.
In Table 2 we give the differences of dDEAB obtained
by fixing either A+ or B which, according to Eq. (17)
should be equal to either D(B%) D(B) or D(A%)
D(A), respectively. From this table we note the following important facts:
1. a remarkable constancy of the experimental values
of D(I) D(I%), irrespective of the nature of the
common ion;
2. that good agreement between the experimental values and those calculated from the electrostatic
model (Eq. (4)) is observed only for large ions such
as OH and Cl whereas there is no agreement for
smaller ions such as H+, Na+, Li+ or K+.
The first point demonstrates that the energy term
(Eq. (18)) is indeed a universal constant, as predicted.
The second point shows that use of an average value of
the dielectric constant is valid only for large ions.
We next give estimates of the coherent energy loss DC
(within the rather large uncertainties in the last column
of Table 2) by using the electrostatic theory for different electrolytes. We obtain for

E. Del Giudice et al. / Journal of Electroanalytical Chemistry 482 (2000) 110116

114

1
1
DCAB = dDE + E(A+) + E(B)
e
e

(22)

the values listed in Table 3. We see that the values agree

within 5% giving an average value of DCAB #6.6 eV
which is some 20% above the result of our simple
calculation (Eq. (18)). This shows again that DC is
indeed a universal constant whereas the electrostatic
interactions are additive and depend on the nature of
the ions: the highly simplified theory which calculates
these energies using screening by an average dielectric
constant is adequate for large ions.
It goes without saying that the approach outlined in
the present paper requires much further development
and that the consequences of the theory need to be
defined and evaluated. The explanation of the primary
dissolution step shows that it should be possible to
interpret the kinetics of reactions in solution in terms of
reaction co-ordinates which include the coherent electrodynamic interactions and this should be equally true
of the kinetics of electrode reactions; furthermore, the
proposed model has important consequences for the
interpretation of the structure of double layers, and
more generally, for the structure of liquid interfaces.
We also note that one important consequence of the
theory is the separation of the apparently homogeneous
solution into domains with different compositions.
These compositional variations should be detectable
both by scattering techniques and by probing the dynamics in sufficiently small systems. Some information
on this aspect is already available. We observe that
semi-permeable membranes (which have holes that are
much larger than the size of both ions and water
molecules) allow the passage of water while the passage
of ions is strictly forbidden (osmosis, reverse osmosis).
Evidently, such membranes select the electrolyte-free
parts of the solution. Ions in their own coherence
domain, which arrive at the membrane, experience a
high electrodynamic barrier. On the other hand, the
small holes which are made in black liquid bilayers by
the insertion of voltage-gated poreformers (for the initial work on such systems, see Ref. [11]) evidently select
the coherence domains of the ions. Further work on the
fluctuations detected in small systems should therefore
allow the development of important new diagnostic
techniques.
5. List of symbols
e
dw

dielectric constant
electric dipole moment of the water
molecule= 1.83 Debyes= 1.15109 cm
(in natural units)
absolute temperature (1 K= 4.31 cm1 in
natural units)

Boltzmanns constant (kB = 1 in natural

units)
N/V
number density of molecules or ions
r
charge density
e
electron charge (e= 0.3, adimensional in
natural units)
a
ionic radius
1/k
DebyeHuckel length
v= 2pn angular velocity, proportional to the frequency n. In natural units 31010 Hz=1
cm1, since the speed of light c =1
2
g
plasma coupling constant
c
molar concentration of the solution
DI
energy loss per ion
kB

Appendix A. The development of quantum

electrodynamics (QED) and the application of this
paradigm to the modelling of electrolyte solutions
As many readers will be somewhat unfamiliar with
the development of quantum electrodynamics (QED),
we are including in this Appendix a brief outline of the
development of this topic of research as related to the
modelling of electrolyte solutions.
One of the major scientific achievements of the 19th
century was the explanation of the laws of gases in term
of Newtonian mechanics and MaxwellBoltzman
statistics and a first step towards understanding entropy
at a microscopic level. However, this freshly constructed topic of classical statistical physics (CP) failed
to account for the newly discovered third principle of
thermodynamics. This failure could be corrected only
by the replacement of the dynamical laws of classical
mechanics by the new concepts of quantum physics,
introduced by Planck, Einstein and Nernst.
Thus, according to the principles of quantum
physics, the systems of statistical physics exhibit a new
type of fluctuation, the quantum fluctuations, which are
non-thermal, and persist when the temperature vanishes. Such intrinsic fluctuations, as we well know, are
precisely those which allow the third principle to hold,
removing the infinities associated with the classical
entropy. The phenomenon of condensation of a Bosegas discovered by Einstein is a particularly enlightening
example of the subtle ways in which quantum physics
Table 3
AB

dDE/eV

D(A+)/eV

D(B)/eV

DC/eV

NaCl
NaOH
KCl
KOH
LiCl

6.61
6.40
6.55
6.35
6.78

0.43
0.43
0.36
0.36
0.45

0.30
0.15
0.30
0.15
0.30

6.74
6.68
6.61
6.56
6.93

E. Del Giudice et al. / Journal of Electroanalytical Chemistry 482 (2000) 110116

explains Nernsts Third Principle. The close relationship of the BoseEinstein analysis of the perfect gas
with Plancks theory of black body radiation brings to
the fore, for the first time, the notion that the only
consistent description of the systems of statistical
physics must be in terms of the fields of quantum field
theory (QFT).
Unfortunately QFT has, until recently, been used
only in the somewhat remote area of subatomic
physics. On the other hand, the every day world has
been interpreted in terms of CP, although the inadequacies of this formalism were already recognised a long
time ago (e.g. by Nernst). The general opinion appears
to have been that CP gives a satisfactory description of
the know-how of matter without any need to investigate the know-why. In the present paper, we have used
a specific topic, the dissolution of electrolytes in water,
to analyse the consequences of abandoning the conventional approach i.e. of replacing CP by QED. The
generally accepted model of electrolyte solutions, the
DebyeHuckel theory, must be incomplete because it is
based on the electrostatic interaction of ions. However,
the dominant term in the motion of ions must be
attributed to Brownian movements (following Einstein)
so that the ions must accelerate and decelerate. The
concomitant radiation (following Maxwell) should
therefore cool the electrolyte to absolute zero at which
point the DebyeHuckel theory would become valid.
We therefore have to ask the question: why does this
not happen? The only possible answer is that the motion of the ions must be rigorously quantised, as rigorously as is the motion of electrons in atoms. Electrolyte
solutions therefore cannot be discussed in terms of any
electrostatic model based on CP: the correct framework
is QED.
We also have to deal with the further difficult question of how we should interpret the interactions of ions
with the solvent. This is discussed currently in terms of
the reduction of the electrostatic interaction of ions by
virtue of the macroscopic dielectric constant of the
solvent. While this can give a reasonable interpretation
of the inhibition of the recombination steps, it cannot
explain dissolution where, as we have already noted in
the main text of the paper, we have to overcome very
high energy barriers to allow the separation of ions
initially present in vacuo in the crystal lattice. We must
also aim to explain a number of further phenomena
such as the increase in the solubilities of most electrolytes with temperature which runs counter to the
decrease of the macroscopic dielectric constant.
We therefore have to consider also the physics of the
pure solvent. In the 19th century it was proposed (on
the basis of arguments such as the increase of solubilities with temperature) that water consists of a mixture
of two fluids whose relative proportions vary markedly

115

with temperature; moreover, only one of these components was presumed to be able to act as a solvent. This
model was abandoned in 1933 when it was pointed out
by Bernal and Fowler that the coexistence of two
distinct phases was forbidden by the indistinguishability
of the individual molecules. However, the two-fluid
model was re-introduced in 1938 to explain the properties of superfluid 4He. The presence of two phases was
now explained as being due to the formation of a
collective state and thermal fluctuations which lead to
the extraction of atoms from this collective state. However, until recently liquid helium has remained an isolated example amongst the assembly of liquids. This
situation has now changed with the application of a
new QED approach to the liquid state based on the
conceptual developments of QFT.
In this new approach, the liquid is shown to be the
final equilibrium state reached by a large ensemble of
molecules oscillating between two specific configurations with an electromagnetic field of frequency n=DE/
h, where DE is the energy difference between the two
configurations, within coherence domains (CDs) having
a radius R= l/2=c/2n = hc/2DE. At first sight such a
metamolecular configuration would require a supply of
a positive energy for the excitation of the electromagnetic field and the atomic excitations; however, this
positive energy is compensated by the negative energy
derived by the interaction of the electromagnetic field
and the current of the large number of oscillating
electrons. Such compensation implies the existence of a
molecular density threshold where the interaction becomes sufficiently large to fulfil the energy requirements. With a further increase of the molecular density,
an energy gain emerges which produces a new minimum energy state at which the system settles at a lower
entropy, The final density is determined by the equilibrium between the electrodynamical attraction and the
short range repulsion between the hard cores of the
oscillating molecules (the size of these molecules is
larger than that of the isolated species). As for the case
of superfluid liquid helium, the collective state is eroded
by thermal fluctuations which produce a non-coherent
fraction of molecules which fills the interstices between
the CDs. On the other hand the CDs experience a
further energy gain by tuning up their respective
oscillations.
We therefore see the formation of an highly non-trivial fundamental state in which the electromagnetic field
and the electron clouds oscillate with a common frequency which is lower than the original frequency
n= DE/h; this mode softening stabilises the state since
it prevents the radiation of the electromagnetic field, i.e.
the minimum energy state is the ground state of the
macromolecular system.
As far as the modelling of electrolyte solutions is
concerned, we need to take note of the fact that the

116

E. Del Giudice et al. / Journal of Electroanalytical Chemistry 482 (2000) 110116

CDs are closely packed sets of molecules which

are basically impervious to solutes; dissolution will
take place only within the non-coherent fraction. We
see that the application of QED leads to a justification
of the two-fluid model developed during the 19th
century. In this paper we have explored the ways
in which the application of this model leads to quantitative predictions for the formation of electrolyte solutions.

Acknowledgements
We wish to thank Professor Roger Parsons for directing us through the archaeology of electrolyte
solutions.

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