Theoretical Foundations of Chemical Engineering, Vol. 34, No. 4, 2000, pp. 301-312.

Translated from Teoreticheskie Osnovy Khimicheskoi Tekhnologii, Vol. 34, No. 4, 2000, pp. 339-352.
Original Russian Text Copyright 9 2000 by Timashev.

CONFERENCE

Science of Complexity: Phenomenological Basis and Possibility

of Application to Problems of Chemical Engineering
S. F. Timashev
Karpov Institute of Physical Chemistry, State Scientific Center of the Russian Federation,
ul. Vorontsovo pole 10, Moscow, 103064 Russia
ReceivedNovember5, 1999

Abstract--The basic principles of flicker-noise spectroscopy, anew method of analysis of chaotic time and
space series, are presented. This method can be considered the phenomenological basis of the currently devel-
oping science of complexity, which deals with open nonlinear dissipative systems of various essences--real
natural objects. The method is based on the postulate that irregularities in measured dynamic variables are of
crucial informational significance in accepting a new hypothesis of scale invariance. In this approach, the power
spectra and the structure functions of different orders are governed by irregularities of various types, namely,
dynamic spikes and jumps of measured variables. For processes under investigation, the expressions for both
the power spectra and the structure functions prove to be identical (invariant) at each of the spatiotemporal lev-
els of the system. The introduced phenomenological parameters completely and unambiguously characterize
the state of the evolving system, thus serving as the "passport data" of the system. The possibility of applying
the proposed methodology to solving topical problems of chemical engineering is discussed.

STATISTICAL ANALYSIS METHODS For example, under various conditions of enhancement

AND SCALING PROBLEMS IN CHEMICAL
ENGINEERING
Modern chemical industrial (catalytic, membrane,
rectification) processes are, as a rule, complex, multi-
step, and multifactor. Information on a process is often
obtained by statistical methods of analysis of the
dynamic variables measured in the experimental inves-
tigation of the process. These methods are aimed at cal-
culating the mean, the variance, and the higher order
central moments [1, 2]. Mathematical modeling of
chemical industrial processes is performed in a similar
manner. It involves an analysis of the macrokinetic
equations of balance (of mass, momentum, energy) for
the studied complex systems with distributed parame-
ters and calculation of the conventionally observed
average chemical reaction rates [3, 4]. Other analysis
techniques, which are employed, in particular, in
designing control systems, seek for empirical regres-
sion models. They can use the information contained in
the spectral densities (periodograms) found from the
time series of measured dynamic variables. However,
in such an analysis, only the characteristic frequencies
indicated by the periodograms are used, and the infor-
mation carried by the continuous portion of the spec-
trum is ignored.
However, experience has shown that the purely sta-
tistical concepts and the account of only resonance fre-
quencies in analyzing the dynamics of complex multi-
factor processes fall far short of being always adequate.
Reportedat the Conf. "Liquid-PhaseSystemsand NonlinearPro-
cesses in Chemistryand ChemicalTechnology,"Ivanovo, 1999.
of the heat and energy transfer in chemical engineering
processes, the kinetics of the observed transformations
is governed not so much by the mean values of the
time-varying dynamic variables (the densities of the
components, the components of the local velocity, etc.),
as by dynamic fluctuations of the local values of these
quantities that are due to the strong correlation between
the motions of neighboring particles or fragments of
the system. In particular, this has been indicated by the
results of the investigation into the dynamics of the
chemical reactions in fluidized-bed apparatuses,
including the study of pulsations of the grain layer den-
sity and the fluidizing flow velocity by various (e.g.,
radiochemical and X-ray) techniques [2]. This infer-
ence has also been suggested by the data from [5-8],
where the optimum operating conditions of fluidized-
bed chemical reactors have been chosen by analyzing
the time series that characterize chaotic motions of dif-
ferent radioactive or fluorescent tracers.
Let us consider one more example of the a priori
insufficiency of pure statistical methods. This example
is related to the modeling of mass transfer (including
that induced electrically) in membrane processes. In
industrial-scale membrane apparatuses, liquid mixtures
are separated by forcing them through narrow (from
fractions of a millimeter to several centimeters in
width) intermembrane gaps. The separating force is
directed perpendicularly to the hydrodynamic flow and
to the membrane surface. This force can be due to the
pressure gradient (in baromembrane processes such as
reverse osmosis, nanofiltration, ultrafiltration, and
microfiltration) or the electric potential gradient (in

0040-5795/00/3404-0301525.00 9 2000 MAIK "Nauka/Interperiodica"

302
Fig. 1. Vortices in a channelof an apparatus in the pulsed
modesof forcingthe liquidmediumat variousarrangements
of baffles [12].
electrodialysis). The main factor that limits separation
in all these processes is the concentration polarization
in the near-membrane surface layers [9, 10]. The con-
centration polarization can be caused by the increase in
the concentration of admixtures. In reverse osmosis
and, partially, in nanofiltration, admixtures are ions;
and in ultra- and microfiltration, they are submicro- and
microcolloidal aggregations able to produce sediments
and to foul pores. In electrodialysis, concentration
polarization can also be brought about by the formation
of the virtually ion-free Nernst layer ~5N in a desalting
cell. However, even at the maximum possible (under
specific process conditions) rates of forcing the liquid
mixture through narrow intermembrane chambers,
when the flow in the bulk of the medium in such cham-
bers can be turbulent, the concentration polarization
cannot be suppressed. For this reason, to enhance mass
transfer, various turbulizers are placed into narrow gaps
(channels) of membrane apparatuses. Turbulizers can
be shaped as grids, corrugated sheets, spirals for swirl-
ing hydrodynamic flows, or curved troughs for produc-
ing secondary flows as pairs of symmetrical vortices
[11]. The widths of these objects are usually chosen to
be from half of the intermembrane distance to the entire
intermembrane distance. In ultra- and microfiltration
apparatuses, the pulsed modes of forcing the liquid
medium are often applied: such modes favor more effi-
cient agitation of the medium in the direction perpen-
dicular to the membrane surface; they also diminish the
deposition of sediments, which foul the pores [12]. The
vortex pattern thereby produced depends on the
arrangement of baffles in the channel of a membrane
apparatus (Fig. 1) [12]. In the near-membrane layers
under such conditions, the mixed (not purely laminar
and not purely turbulent) flow takes place.
In electrodialysis of diluted electrolyte solutions
(at solution concentrations C < 0.005 M), when the
task is to obtain deionized water with the resistivity
1-10 mf~ cm [13, 14], turbulizers become inefficient
[14], and the mass transfer is enhanced by applying
anomalously high densities of the electric current J,
which considerably exceeds the limiting diffusion cur-
rent Jlim"
THEORETICALFOUNDATIONSOF CHEMICALENGINEERING Vol. 34
TIMASHEV
Of course, model calculations of the hydrodynamic
flows in narrow channels with turbulizers and various
inserts are difficult to perform; and with allowance made
for concentration, temperature, and current inhomogene-
ities in real membrane apparatuses, these calculations
are impossible. However, for computing the transmem-
brane flows of various components in membrane appara-
tuses, such information is necessary. The enhanced (by
using turbulizers or overcurrents) mass-transfer through
membranes is commonly characterized by the Sherwood
number Sh = km/k~ where km and k~ are the enhanced
and unenhanced mass-transfer coefficients, respectively
[10, 14]. Representations of the Sherwood number Sh
are chosen with regard for the specificity of each individ-
ual problem. In some ranges of the Reynolds number
Re = MAt and the Schmidt number Sc = v/D, the follow-
ing relation is valid, which relates these numbers to the
Sherwood number Sh computed from the observed
mass-transfer data [10, 14]:
Sh = ARemScn. (1)
Here, A is an empirical constant found for each type of
apparatus, m and n are phenomenological parameters
determined by fitting experimental data for different
modes of flow with the characteristic velocity u along a
channel of the characteristic size 1, v is the kinematic
viscosity, and D is the diffusion coefficient.
In examining the hydrodynamic flows in channels
of apparatuses and the transmembrane transfer in elec-
trodialysis, the following expression for the Sherwood
number is used [14]:
Sh = J|iml(tm- t~)I(CDF), (2)
where tm and t~ are the transport numbers of counteri-
ons in the membrane when the current density is close
to its limiting value, and in the electrolyte, respectively;
i = 2h; h is the channel width; and F is the Faraday num-
ber. According to [14], in the case under investigation,
m = 0.5 and n = 1/3.
These concepts are adequate in considering the elec-
trically induced mass transfer during electrodialysis in
apparatuses with a relatively large intermembrane dis-
tance. This follows from Fig. 2 [14], which presents the
dependence of Sh on Re in electrodialysis for channels
with geometrically similar grid separators of various
thicknesses, which are the most efficient ones for nar-
row channels. At h > 1-2 mm, relation (1) with the
above values of the parameters m and n is obeyed;
whereas at h < 1 mm, it is violated because of the rela-
tive enhancement of the wall effects, which abruptly
suppress the mass transfer. This gives rise to two issues.
One of them is that criterial relations, which are often
used in chemical engineering for solving scaling prob-
lems, may sometimes be invalid. Therefore, one should
either correct these relations (in the above instance,
relation (1) should probably be supplemented by one
more characteristic dimensionless parameter as a fac-
tor, with the following experimental verification) or put
No. 4 2000
 SCIENCE OF COMPLEXITY: PHENOMENOLOGICAL BASIS
forward other methods for solving scaling problems.
The other issue is the necessity for finding new ways
and means of mass transfer enhancement during elec-
trodialysis in apparatuses with narrow channels,
because purely hydrodynamic means (raising the Rey-
nolds number Re) turn out to be inefficient. Such
approaches are now known [13, 14]. They involve
applying anomalously high (as compared to that
applied in earlier practice) current density, which, as
noted above, can substantially (tens of times in elec-
trodialysis of diluted electrolyte solutions) exceed its
limiting value. However, analysis of the phenomena of
the hydrodynamic instability caused by the passage of
the high-density current through a system has shown
that the conditions of inducing these effects are difficult
and rather impossible to represent in the conventional
dimensionless form, namely, as the dependence of Sh
on an empirically (intuitively) found set of characteris-
tic dimensionless parameters. Introduction of integral
(throughout the channel or the membrane surface) cri-
terial parameters proves to be a priori insufficient. It is
such parameters that are usually introduced in model-
ing chemical engineering processes on the basis of
information obtained by statistical methods. As for
local (point) values of the dimensionless parameters,
they are of little use in industrial process design, and
much less, in solving the scaling problems.
DETERMINISTIC CHAOS: A NEW PARADIGM
OF CHEMICAL ENGINEERING?
New possibilities of solving problems of modeling,
control, and prediction of changes in the states of open
dissipative systems in chemical engineering have been
opened up by the application of methods of the nonlin-
ear dynamics and the deterministic chaos theory [15-
17]. General ideas of applying the principles and mod-
els of the nonlinear dynamics of dissipative systems to
complex multifactor chemical industrial processes, in
particular, to catalytic processes, have been discussed
for a long time [ 18]. Formulating adequate models of
such processes is an extremely complicated problem.
For example, a mathematical model of natural gas com-
bustion considers 196 forward reactions and the same
number of reverse reactions, which involve 32 compo-
nents. At the same time, the nonlinearity of relation-
ships in a dissipative system with as few as three
degrees of freedom can give rise to a chaotic mode, in
which the evolution of the system is sensitive to the
choice of the initial conditions, and the trajectories of
the system in the phase space asymptotically approach
a certain set--a strange attractor [15]. The strange
attractor has fractional dimensions and zero volume in
the phase space with integer dimensions, although its
domain of attraction has nonzero finite (or even an infi-
nitely large) volume. Such are the most important prin-
ciples of the modem science of deterministic chaos.
One should note here the fundamental difference
between frictional (dissipative) and frictionless (con-
THEORETICAL FOUNDATIONS OF CHEMICAL ENGINEERING
303
Sh m 1
"2
102 9 4
i
v5
100 101 102 103 Re
Fig. 2. Dependences Sh(Re) for geometrically similar grid
separators: the grid mesh is square-shaped; the ratio of the
step of the grid to the grid thickness is 3; the channel length
is 0.4 m; the channel height is equal to the grid thickness
h = (1) 1 l, (2) 6. l, (3) 3. l, (4) 2.0, (5) 0.8, (6) 0.46, (7) 0.26,
and (8) 0.18 mm [14l.
servative or Hamiltonian) systems. It is the presence of
the internal friction (in the broadest sense) that entails
the existence of the attractor as the asymptotic limit (at
t , oo, where t is time) of the solutions, the limit that
is not affected directly by the initial condition: in the
course of their evolution, trajectories that correspond to
different initial conditions outside the attractor "settle
down" in the attractor (for more details, see [15, p. 135]).
All this means that it is still premature to talk about for-
mulation of adequate models, i.e., models that would
correctly represent the basic relationships in the above
complicated chemical transformations. Moreover, in
actual chemical process cycles, such transformations
often occur under no less difficult-to-model heat- and
mass-transfer conditions, in particular, in turbulent
flows, as in fluidized-bed apparatuses. This raises the
question: if one cannot access the possibility of ade-
quately describing complex dissipative chemical engi-
neering processes with large numbers of degrees of
freedom, then on what basis and how can one solve the
challenging problems of optimum organization of such
complex processes and the problems of scaling-up lab-
oratory apparatuses to industrial ones.
Of course, one can refer to the rich experience of
practical industrial engineers, who have succeeded in
designing quite efficient chemical engineering pro-
cesses without serious mathematical modeling. But
what is the true cost of such designs with regard for the
inevitable "spoilage embodied in metal," and what will
be their true efficiency and the energy- and resource-
saving characteristics if we take into account the com-
plex character of any industrial production?
This is the reason why, recently, the methods of non-
linear science have been introduced into the practice of
Vol. 34 No. 4 2000
304 TIMASHEV
analysis of chemical industrial processes. In particular,
it was inferred [5-8] (see also [19]) that the problems
of scaling fluidized-bed reactors can be solved only by
analyzing time series and finding the parameters of
dynamic state of the chaotic flows in these reactors.
According to [5-8], as these parameters of state, one
can take the characteristics of the power spectra of the
measured dynamic variables [15] and also the dynamic
entropy, which characterizes the loss rate of informa-
tion in turbulent flows [ 16, 17].
How suitable are the methods of the nonlinear
dynamics and the deterministic chaos theory for solv-
ing the above problems? One more circumstance
should be taken into account in discussing the potenti-
alities of employing the theory of dissipative dynamic
systems and deterministic chaos for adequate analysis
of information obtained in experimental investigation
of physicochemicai and chemical industrial processes.
The existing methods of the nonlinear time series
analysis [16, 17] and the procedures of extracting infor-
mation on the evolution of an open dissipative system
from the time series of the measured dynamic variables
V(t) are based on the assumption that it is possible to
introduce a multidimensional phase space containing
the trajectory of the dynamic process examined [15-
17]. It is assumed that the measured variable reflects the
total dynamics of the system well and that the topology
of the attractor can be reconstructed from the results of
observation of V(t) only. In each specific case, the ques-
tion arises of how many dynamic parameters should be
taken for unique characterization of the flows occurring
under given conditions. Apparently, the required meth-
odology of analyzing the dynamic state of complex sys-
tems should provide the possibility of introducing an
arbitrary number of dynamic parameters, each having
quite a definite physical meaning to serve as a physical
parameter of the monitored chaotic flow. From this
standpoint, the nonlinear time series analysis [15-17] is
a priori restricted. This methodology considers a lim-
ited number of parameters extracted from the time
series, viz., the attractor dimensions, the Poincare sec-
tion characteristics, the Lyapunov exponents, and the
Kolmogorov entropy.
Another comment should be made concerning the
above initial postulate of the methodology under dis-
cussion [15-17], according to which any time series to
be analyzed corresponds to a process that, in principle,
can be represented adequately by a finite (and not very
large, because the deterministic chaos is considered!)
set of differential equations. This postulate appears
very controversial as far as the dynamics of real pro-
cesses is concerned. Let us illustrate this point by the
example of the dynamics of crystallization of some
substance from a supersaturated solution. Let us select
a structural fragment on the surface that is characteris-
tic of a certain selected spatiotemporal scale of the sys-
tem, and let us imagine the structural transformation of
this fragment during crystallization. Obviously, the
THEORETICAL FOUNDATIONSOF CHEMICALENGINEERING Vol. 34
measured (at this level of organization of the system,
i.e., by instruments with a certain magnification)
change of this fragment (with the formation of, e.g., a
new element by the phase transition (crystallization) in
some region of the chosen fragment) proceeds in a cer-
tain finite (and characteristic of the organization level
considered) time interval. In shorter time intervals,
there occur structural transformations (phase transi-
tions) at lower levels of the system organization, which
are not detected at the selected level. Apparently, differ-
ential equations (if their number is finite) cannot
describe this crystallization dynamics, especially when
the multilevel structure of the system is taken into
account. That is why it is not surprising that, in analyz-
ing actual time series (obtained by experimental inves-
tigation of some processes rather than from a set of
nonlinear differential equations!), the methodology
under discussion [15-17], as mentioned above, has not
yet led to any noticeable success.
Below, we present a new phenomenologicalapproach
to the extraction and analysis of the information con-
tained in the chaotic time and space series, which char-
acterize the evolution and the structural organization,
respectively, of open dissipative systems of various
natures [20-29]. This approach, referred to as flicker-
noise spectroscopy, can be considered the phenomeno-
logical basis of the currently developing science of
complexity, whose objectives are beyond the scope of
the deterministic chaos theory with analysis of finite
sets of nonlinear ordinary differential equations.
FLICKER-NOISE SPECTROSCOPY
AS THE PHENOMENOLOGICAL BASIS
OF THE SCIENCE OF COMPLEXITY
The approach elaborated in [20-29] is based on the
systemic view on the science of complexity, on the evo-
lutions of open dissipative systems with nonlinear
interactions between elements of systems and sub-
systems, and on the formation dynamics of complex
spatial patterns during passage of energy and mass
flows through a developing system with nonlinear
interactions between its fragments of different spatial
scales. The systemic character of the methodology
implies, first of all, two basic ideas: the idea of hierar-
chical order (for the spatiotemporal levels of the inter-
nal organization of a system) and the idea of informa-
tional significance of irregularities in measured
dynamic variables.
The starting point of flicker-noise spectroscopy is
the fundamental irregularity (revealed from various
time series) of the space and time dependences of the
dynamic variables h(x) and V(t) measured for industrial
and natural processes of various natures. This irregular-
ity manifests itself in abrupt jumps of h(x) and V(t),
with the jump magnitudes varying over wide ranges.
Moreover, after having been scaled up, each of the frag-
ments of such evolutionary dependences, even for
steady processes, exhibits the same type of irregular
No. 4 2000
 SCIENCE OF COMPLEXITY: PHENOMENOLOGICAL BASIS 305

i_l~ -." ! .... -~

I I I I I I
I I I I I | /
I I I I I ~ I I
I I I I I |
I I I I I I ~ I
I I I I 9 I I ii i i i ,,~ j
I I I I T I I l T
I I t t / I I L -1 I I I I I I iI ~"
I I I I I I
i i , t / II II I I I I I I I I
I I I I / I I I| I I I I I I I I I
, i , 'V II ,I I I I I I I I I "'"
I I I I I I I1 I I I I I I I I I
I I I I I I I ~ , I I I I I I I I I
I I I I I I I ~ " .... 9 I I I I I I I I I I
I I I I I I I I I I I I I I I I I I
I I I I I I I I I I I I I I I I I I
' I I ! !! ! ' ' ' I I I I I I I

"lk*(l) "0k'(l) "0k'(2) 'o~t93tlk(2)t~k"+l) '0k'(i)"it'(3) t(i+l)0~ "lk~ t0t'(m) 10k

,(m+l) ,(5)
61k

Fig. 3. Hypotheticalfunctionrepresentingof the evolutionof the dynamicvariable [20].

behavior (see [21 ]). This character of the evolution sug-
gests that not all of the points in the space or time axis
are equivalent with respect to information significance.
For definiteness, let us further examine only the
time series V(t), assuming that, for the space series h(x),
the character of all the dependences to be obtained
below is the same. In time intervals that are character-
istic of a certain (ith) spatiotemporal level of evolution,
there exist some short ~5 intervals that carry the main
information on the structure--energy state of the system
under investigation. The widths of the time gaps
between these 5 intervals prove to be of information
significance as well, and on each of these time gaps,
there can also occur short ~5intervals at a lower tempo-
ral level that contain information on the state of the sys-
tem, and so on. Within each of such sequences, there
are correlations of various types (see below) between
the measured dynamic variables, and the parameters
characterizing them carry information on the dynamic
state of the considered nonlinear system. The transition
of the system from one information-significant state
into another one that differs in structure-energy charac-
teristics is reflected by the change in the value of the
dynamic variable V(t) and is fixed at the moment when
this transition becomes irreversible.
To materialize these physical ideas and elaborate the
time series analysis methodology on their basis, one
needs to idealize the introduced representation and to
contract all the information-significant {i intervals at
various ith spatiotemporal levels into points. Each of
these points (instants) should be a carrier of informa-
tion on the structure-energy state of the system at this
moment of time, i.e., should be a marker of irregulari-
ties of various types in the system. The zero duration of
each of the instants means that the value of the studied
function at each of these points should contain an
(actual or potential) singularity, i.e., should be repre-
sentable as the sum of a zero-support generalized func-
tion [30] (expressed as the sum of delta functions and
their derivatives) and functions with discontinuities of
different types (the Heaviside theta function and func-
tions with derivative discontinuities of the first, second,
and higher orders). One also needs to relate the evolu-
tionary changes in the considered system at various
spatiotemporal levels by some scaling relations. This
can be done by introducing certain invariants of the
process in analyzing the effective densities of irregular-
ities of each type (see below). Thus, an idealized model
function V(t) is introduced (Fig. 3), and it is assumed
that all the main information on the evolutionary pro-
cess is contained only in the above singularities and dis-
continuities of this idealized function, which are
regarded as the main and only markers of the evolution-
ary process.
The evolution of the dynamic variable V(t) at the ith
spatiotemporal level is postulated to have the most gen-
eral intermittency form. Such an evolution is character-
ized by comparatively small changes in relatively long
time intervals (laminar phases) of characteristic dura-
tion T0, being abruptly interrupted by short spikes of
duration x0i (,c0 ,~ To ). During the spikes, there occur
jumps of the dynamic variable on the next laminar
interval, which are accompanied by derivative break-
ing. Let us assume that the jumps and discontinuities
are of the first kind and that the variable V(t) can exhibit
abrupt jumps (on short intervals of duration "oil) of the
laminar background (Fig. 3). Let us suppose that these
abrupt jumps are of the second kind, and let us desig-
nate the characteristic time intervals between these
abrupt jumps by Ti! (it is taken that 17il "~ Til ). The
acceptance of the hypothesis of scale invariance means
that a similar evolution proceeds in the temporal region
as well (Fig. 3, dot-and-dash line); i.e., it means that the

THEORETICAL FOUNDATIONSOF CHEMICAL ENGINEERING Vol. 34 No. 4 2000

306 TIMASHEV

general form of the temporal evolution with the spikes
and the jumps of the dynamic variable remains the
same at each of the spatiotemporal scales of the evolu-
tion under consideration.
This representation of the model function V(t)
enables one to obtain (using some theorems of the the-
ory of generalized functions) relatively simple analyti-
cal expressions for dependences that are usually calcu-
lated from experimental time series in order to find the
phenomenological parameters of the studied dynamic
system by collating the theoretical and experimental
relationships. For this purpose, the power spectrum is
analyzed, which is the spectral density S(f) ( f is the
frequency) of the autocorrelator
spikes have been subtracted from the dependence V(t)
but the jumps of the dynamic variable have been
retained). Then,
S ( f ) = Ss(f) + SR(f),
~. (7)
SR(f) = 2~cos(2~f'O ( VR(t)VR(t + "O)d'c.
o
In the low-frequency limit 2nfT~ ,~ 1, the dependence
Ss(f) at the ith spatiotemporai level, which is given by
only the singular term Vs(t), i.e., by the spikes of the
dynamic variable V(t), takes the form

~('c) = ( V ( t ) V ( t +'c)) (3)

Ss(f) = 2~O0(rl)cos(2T0frln)drl, (7a)
of the measured dynamic variable:
0

S ( f ) = 2~cos(2~fx)~(x)dx, (4) where the introduced function O~ characterizes the

o
~t(x) = 2 I c o s ( 2 x f x ) S ( f ) d f . (5)
0 roZo(bdl),
Here, the W(x) = V(-x) steady processes are considered,
the angle brackets ( ) mean the averaging over the ini-
tial time t, and it is supposed that (V(t)) = 0. The differ-
ence moments O~,)(x) (the structure functions in the
theory of developed turbulence) of different orders p
have the form
effective (with regard for the spike amplitudes) spike
density in the evolution. In accordance with the dimen-
i
sion V2t of the function ~0 (z), one can write
(8)
where x0(b~rl) is a dimensionless function, b~ is a
dimensionless scaling factor at the ith spatiotemporal
level, and g is a constant with the dimensionality I/2.
Then,
oo

9 ~p)(X) = ( [ V ( t ) - V(t + x)]P), (6)

Ss(f) = g fXo(X)cosZxdx,
KO~./ (9)
where x is the time interval between two analyzed val- 0
ues of V(t). It is known that the independence of the i i
spectral density S(f) of the frequency throughout the Ko =-bolTo, Z - 2 frclK o.
frequency range (the so-called white noise), as well as Here, a scale-invariant parameter K0 is introduced,
the independence of the difference moments ~q,)(x) of
which is independent of the number of the spatiotem-
the delay time x, suggests the absence of correlations poral level. That is, it can be regarded as an invariant of
between preceding and subsequent events. However, in the process under investigation. For the function x(Z),
each individual case, one should check and specify one should choose approximations that adequately rep-
what characteristics of the evolutionary processes are resent the possible types of the prolonged nonexponen-
correlated. In the methodology under discussion, these
tial nonlinear relaxation in the considered systems,
distinguishable characteristics constitute the irregulari- which is accompanied by probable structural rear-
ties examined, and the parameters introduced below rangements [20, 27]:
will be defined in terms of combined properties of the
moments of time and the amplitudes of the irregulari- the flicker-noise approximation,
ties considered to describe the rate of loss of the corre-
lations in the sequence of the markers. x ( Z ) = Z -~t, O < i t < l ;
Let us consider the evolutionary dependence V(t), the Levy approximation,
which characterizes the time changes at the ith spa-
tiotemporal level. According to [22], to deduce the x(Z) = exp[-(Z,oZ)S], 0 < s < 2;
expression for the power spectrum S(f), the signal V(t)
is conveniently represented as the sum of two terms: the the modified Levy approximation,
singular term Vs(t) (which is determined by the spikes x(Z) = exp[-O.oZ) ~- (VoZ)q], 0 < s < 2, q > 2,
of the dynamic variables) and the regular term VR(t) =
V(t) - Vs(t) (which is the remainder that is left after the where It, ~o, Vo, s, and q are parameters.

THEORETICAL FOUNDATIONS OF CHEMICAL ENGINEERING Vol. 34 No. 4 2000

 SCIENCE OF COMPLEXITY: PHENOMENOLOGICAL BASIS
Note that the inequality 0 < s < 2 in both Levy
approximations (the second and third cases) ensures the
positive definiteness of the function Ss(f) at m = v0fL0 ~
1 and q = 2-4. According to [20, 27], in the flicker-noise
approximation,
Ss(f ) _ if(1 - It)
In the Levy approximation, in the limit
f ' ~ f0 -- ~,0K0/(2n)
the power spectrum is frequency-independent (the
"loss of memory" at times longer than tm~ f01 ); and
with increasing frequency, it decreases according to a
power law a s f ~ with n = s + 1 and 1 < n < 3 in the fre-
quency range j~ '~ f '~ K0/(2n). In the modified Levy
approximation, the power spectrum is also frequency-
independent a s f ,. 0 and diminishes with raising fre-
quency as f-n; but in this case, the parameter n exceeds
the above value n = 3 in the high-frequency approxima-
tion and can vary throughout the possible range of n if
q - 2-4. Note as well that, in the Levy approximation,
one can obtain an analytical expression for Ss(f) at s =
0.5 and 1 (see [20]).
Apparently, the dimensionless parameter n charac-
terizes the degree of loss of correlations in the spike
sequence with allowance made for the spike amplitudes
in relatively short time intervals (At ,~ tm - f01 ). The
Levy approximations demonstrate new possibilities of
describing irregularities of evolutionary processes by
introducing a new type of self-similarity in them. This
self-similarity is related to correlations between irregu-
larities of only one type, namely, spike sequence. These
correlations are characterized by not a single phenom-
enological parameter (as for fractals), but by several
(two or more) ones. Note also that relation (9) implies
that Ss(f) - 0 if these is no correlation in the spike
sequence, i.e., if the Poisson distribution is observed at
I1 , 0, s - 0, and ~ ,. 0. Obviously, the lower
the frequencyfthe larger the number of spatiotemporal
levels at which the inequality f , ~ 1/(2reT~ ) is valid.
For practical determination of these phenomenolog-
ical parameters, instead of analyzing the Levy approx-
imations of general relations (9), one can analyze the
interpolation expression
1
Ss(f) -- Ss(O) 1 + (2nT0f)"' (10)
where, along with T-~01 - ~ K 0 and n, an effective phe-
nomenological parameter Ss(0) of the process is intro-
duced.
Equations (9) and (10) give the first set of invariant
parameters, which describe the self-similarity of the
most abrupt irregularities of the evolutionary process,
specifically, the sequence of dynamic spikes. However,
THEORETICAL FOUNDATIONS OF CHEMICAL ENGINEERING
307
for finding these phenomenological parameters from
the power spectra computed from the experimental
time series, one needs to derive the dependence SR(f),
which can be done by the expression for 0(2)(0:
oo
SR(f) = ~cos(2~fx)[O(2)(~176 (9a)
0
As shown in [20-22], the dependences O~,)(t) are
defined only by the jumps of the dynamic variable V(t).
The simplest interpolation dependence for the differ-
ence moments of order p in the case when the contribu-
tion of the second-type jumps is negligible has the form
r = gl(p)~P[ 1 - F-1(HI)F(HI, Tlllt)] p, (11)
where ~ is the variance of the dynamic variable V(t);
2 = (1/2)O(2)(oo);
gl(P) is a parameter that characterizes experimental val-
ues of tI)(p)(Oo)(gl(2) = 2); ~ l = ~,lKl is a phenomeno-
logical parameter that describes the time interval in
which the information on the value of the dynamic vari-
able is completely lost and that is determined by a
model parameter ~,~ and the second scale-invariant
parameter K1 of the process [20-22]; H l is the Hurst con-
stant; and F(s) and F(s, x) are the gamma function and
the incomplete gamma function, respectively (x > 0,
s>0).
When the contribution of the second-type jumps
cannot be neglected, a more general interpolation
dependence should be used:
O(p,(t) = gI(p)IfP[G(HI, 1 ) + T~G(H2, T~12t)
Tlllt 1 ] P(12)
,
G(H/, LTTl~t ) - 1 - r-'(nj)r(nj, TTl~t), j = 1, 2,
where the subscripts j = 1 and 2 refer to the parameters
of the first- and second-type jumps, respectively; t~j is
the variance of the dynamic variable V(t) because of the
variation in the jumps of the jth type [(I)(2)(oo ) ---- 2(ol +
o2)2]; Hj is the Hurst constant that describes the average
rate of change in the value of the dynamic variable
owing to the occurrence of the jumps of the jth type in
the time intervals shorter than the correlation time Tlj;
and T is the parameter that characterizes the relative
contribution of the second-type jumps.
Equations (l l) and (12), along with more general
expressions [20], can be used to obtain information on
the phenomenological parameters H 1 and ~,IKI of the
studied system by collating these dependences with the
corresponding expressions derived from the observed
time series. Note that the second-type jumps should
contribute to the dependences O(p)(t) on long time inter-
vals at t >> T1. In this instance, one should introduce
additional parameters HE and ~ K 2. Equations (11) and
Vol. 34 No. 4 2000
308
(12) give the second set of invariant parameters, which
describe the self-similarity in the dynamics of the loss
of memory about the values of the variable V(t) at some
fixed moments of time during the evolution. This
dynamics is completely realized through the jumps of
the dynamic variable, The corresponding phenomeno-
logical parameters are found by collation of the differ-
ence moments of various orders that are calculated
from experimental time series, with (11), (12), and
more general formulas presented in [20].
One can readily check that the dependence SR(f)
obtained by substituting (11) into (9a) can be approxi-
mated by the function
1 to the identity 0 --- 0 at a certain step of differentiation
SR(f) = SR(O)
1 + ( 2 n T l f ) 2n'+l'
whose parameters generally differ from the respective
parameters of equation (10):
SR(0 ) =/=Ss(O), TII ! = ~ I K I r 2HI ~=n- 1.
Collation of the power spectra found from experimen-
tal time series with general phenomenological relations
is conveniently performed when, according to (7), the
total spectrum S(f) is represented as the sum of inter-
polation expressions (10) and (10a). The corresponding
analysis allows one to separate (in each individual case)
the contributions to S(f) that are due to different irreg-
ularities (the spikes and the jumps of the dynamic vari-
able), and to determine the values of the parameters
introduced above.
Let us elucidate the meaning of the parameters
obtained by comparing relations (10)-(12) with the
corresponding dependences calculated from experi-
mental time series by presenting the parameter values
in some well-known special cases:
The Fick diffusion,
2H=l, n = 2 H + 1 =2;
The Levy diffusion,
2H=s, n = s + l , 0<s<2;
The enhanced diffusion,
1 / 2 < H < 1;
The diffusion with geometric constraints,
H < 1[2;
The modified Levy approximation,
H>I, n = 2 H + 1>3;
The fully developed turbulence (the Kolmogorov-
Obukhov law),
2H = 2/3, n = 2H + 1 = 5/3;
The turbulent diffusion (a passive particle in a turbu-
lent flow),
2H=3, n=2H+l=4.
THEORETICAL FOUNDATIONS OF CHEMICAL ENGINEERING
TIMASHEV
Collation of the parameters found by analyzing the
time series with those determined in these special cases
enables one to represent (albeit qualitatively) the char-
acter of the complex processes that exhibit the studied
evolution.
Note as well that additional information on the evo-
lution of V(t) is contained in its time derivatives dmV/dt'n
of various orders m (m > 1). From the derivative of each
order, the Fourier spectrum Stm)(f) of the correspond-
ing autocorrelator and the difference moments --p ~c,~)('0
are computed [20-22]. The proposed procedure of
determination of the parameters proves to be conver-
gent, since successive differentiation necessarily leads
(10a)
and, as a consequence, to limitation of the total number
of the process parameters.
The methodology of flicker-noise spectroscopy has
previously been used for determining the "passport
data" of a number of surface patterns and natural tem-
poral processes: the roughness of the surfaces of cata-
lysts and ceramics, fluctuations of the electric voltage
in electromembrane systems and semiconductors, fluc-
tuations of the local rate constant in the chemical and
electrochemical kinetics, fluctuations of the compo-
nents of the velocities of turbulent flows, and variations
in the solar wind parameters and in the stratospheric
ozone concentration [23-28]. Given below is one of the
examples of such an analysis of complex signals repre-
sented as time series obtained in electrochemical exper-
iment in order to extract the general phenomenological
information on the system under investigation.
EXAMPLE OF APPLICATION
OF THE METHODOLOGY
OF FLICKER-NOISE SPECTROSCOPY:
ANALYSIS OF THE DYNAMICS OF POROUS
SILICON FORMATION UNDER ANODIC
POLARIZATION [24, 28]
Porous silicon is produced by electrochemical treat-
ment of single-crystalline silicon in hydrofluoric acid
solutions under anodic polarization during simulta-
neous occurrence of many complex and still incom-
pletely understood processes, both physical and chem-
ical, including morphological transformations of sili-
con. Anodic treatment of n-Si and p-Si demonstrates a
great difference between the characters of the measured
potential fluctuations under the galvanostatic operating
conditions, which suggests the differences in mecha-
nism of porous silicon formation between these
instances. The characteristics of porous silicon sam-
ples, in particular, the pore size distributions and the
noise power spectra, turn out to be very sensitive to the
choice of the electric current density used in the porous
silicon synthesis. Below, we present some results of
investigation of the noise characteristics of the electric
potential at various measured electric current densities
[24, 28].
Vol. 34 No. 4 2000
 SCIENCE OF COMPLEXITY: PHENOMENOLOGICAL BASIS 309

U,V
(a)

ill

3
_ _ 1 II i -- -

ii i
2 i

w
1
I I I I I I I I I t

0 2 4 t X 10-2, s
U,V

(b)

0.2

0.1
3

I I I I I I I I I I

0 2 4 t x 10-2, s

Fig. 4. (a) Time dependencesof the potential of the platinumanodeunder anodicpolarizationof n-Si in a 30% HF solutionin ethanol
during simultaneousexposureto light emittedby a 100-Whalogenlampat the electriccurrentdensityi = (1) 10, (2) 20, (3) 50, (4) 75,
and (5) 100 mA/cm'; (b) those after subtractionof the slowlyvaryingcomponentof the anodicpotential.

Figure 4a displays the time dependences of the
anodic potential, which reflect the formation kinetics of
porous silicon at different electric current densities
under simultaneous photoexcitation by a halogen lamp.
Figure 4b shows the same dependences after subtraction
of the slowly varying component of the anodic potential.
The measured potential fluctuations become stronger
with rising operating values of the electric current den-
sity. The task is to describe the measured qualitative dif-
ferences between the recorded signals by a quantitative
expression in terms of the methodology of flicker-noise
spectroscopy. For this purpose, Figs. 5 and 6 give the
dependences S(f) and (I)t2)(x), respectively, that are cal-
culated from the measured time series at two values (10

THEORETICAL FOUNDATIONS OF CHEMICAL ENGINEERING Vol. 34 No. 4 2000

310 TIMASHEV
(I)(2), V2
S, V2/Hz (a)
(a)
10-4

10-5

10-6

10-7
10-6
/
/

I I i Illlll I [ I IIIIII I I I IIIIll I I I IIIIII IIII I I I IIIIII I I I IIIIII I I I IIIIII I I Ill

10-3 10--2 10-1 100 f, Hz 10 -l 10 o 101 102 I;, s

(I~(2), V 2
S, V2/Hz 10-3
(b)
10_11 - - . ~ , (b)

10-2 I

10-3 IL

10-4 I 10-4

10--5~ I I I IIIIII I I I IIIIII I I I IIIIII I I I IIIII II [ I I Illll | I I IIIlll I I I I Illll I I I

10 -3 10 -2 10 -1 100 f, Hz 10 -1 10 o 101 10 2 %S

Fig. 5. Power spectra for the anodic proces_s in Fig. 4: (a) Fig. 6. Second-order difference moments for the anodic pro-
the electric current density i = 10 mA/cm z, S(0) = 5.2 • cess in Fig. 4: (a) the electric current density i = 10 mA/cm 2,
10- 5 V 2/ H z , TO = 4.3 s, and n = 1.25; (b) i = 100 mA/cm 2, o=7.1 x 10-4 V, H = 0.09, and T1 =5.8 s; (b) i= 100 mA/cm 2,
Sl(0) = 1.1 x 10-3 V2/Hz, $2(0) = 4 • 10-2 V2/Hz, TOl = o = 0.012 V, H l = 0.45, T! 1 = 3.3 s, H 2 = 1.0, Tl2 = 66.1 s,
0.32 s, T02 = 11.4 s,n I =2.27, andn2=2.17. T = 0.32.

and 100 mA/cm 2) of the electric current density. The fig- scales of irregularities--jumps and spikes. This cir-
ures also present the above-introduced phenomenologi- cumstance should be taken into account by the models
cal parameters found from these dependences. of the system under exploration.
Analysis of Figs. 5 and 6 revealed that, at low cur- The aforesaid means that flicker-noise spectroscopy
rent density, the integral duration of the "memory" is shows itself as a true spectroscopy, disclosing the dif-
greater (the To values are larger). An increase in the cur- ferences between the mechanisms of the process under
rent density raises the rate of loss of the memory (n investigation at various current densities by analyzing
rises to 2.2) and gives rise to a two-component spec- the noise spectra. This information has not hitherto
trum (in Fig. 5b, two steps at low densities emerge). been obtained by other methods. It can provide a better
The dependence ~(2)(x) also becomes two-component understanding of the variety of complex chemical and
as the current density is raised (Fig. 6b). Apparently, the electrochemical reactions occurring in the formation of
increase in the current density above a certain threshold porous silicon.
induces some extra electrochemical processes which
do not occur at low current densities. From the stand- CONCLUSION
point of general phenomenology, and in light of rela-
tions (12) and (12a), the emergence of the second com- The results obtained suggest that, currently, there is a
ponent in the dependences S(f) and ~(2)(x) points to need for the reform of chemical engineering education
significant effects associated with two characteristic that would involve the abandonment of not only the con-

THEORETICAL FOUNDATIONS OF CHEMICAL ENGINEERING Vol. 34 No. 4 2000

 SCIENCE OF COMPLEXITY: PHENOMENOLOGICAL BASIS
ventional statistical concepts of processing of data col-
lections (ensembles) obtained in physicochemical inves-
tigations or real technological processes, but also the
notions of the nonlinear dynamics and the deterministic
chaos theory in their classical formulations.
As Prof. Nalimov has noted in his preface to Him-
melblau's classical monograph [1], the previous great
reform of engineering education with an emphasis on
introducing the probabilistic methods of data process-
ing was carried out in the 1970s under the undoubted
influence of this monograph. The transition to "nonlin-
ear thinking" has not been performed completely,
which is likely to be due not only to the apparent diffi-
culties in analyzing sets of nonlinear ordinary differen-
tial equations (see the above comments to [18]) but also
to the inadequacy of these sets of equations to actual
complex processes (which has also been discussed).
Probably, it is due to this inadequacy that works on
application of the nonlinear time series analysis to real
technological processes with determination of more
than one parameter are very few.
At the same time, the time series analysis methodol-
ogy presented in this work allows one to characterize
any complex process on the time intervals of its quasi-
steadiness with a required degree of individualiza-
t i o n - f r o m the topochronological parameters. These
phenomenological parameters have quite a definite
physical meaning and are regarded as the "passport
data" of the studied system. The introduction of such a
parametrization of the dynamic state of a complex mul-
tifactor system will possibly enable one to advance in
solving chemical engineering problems (including the
scaling problem) that are unsolvable by the conven-
tional methods. Note that I am not alone in suggesting
such ideas (see [5]).
There are two main "sources" of the introduced def-
initeness of the parameters of state. The first of them is
the accepted postulate of a multitype, "colored" charac-
ter of the input information, which is due to the associ-
ation of the information with various irregularities of
the studied signal. The second is the multiparameter
self-similarity of the evolutionary dynamics of open
nonlinear dissipative systems, which means the resem-
blance between the laws of the chaotic dynamics at all
the spatiotemporal levels of the investigated system.
From this standpoint, one can understand the origin of
the failures of the existing nonlinear approaches to ana-
lyzing chaotic series; in particular, in calculation of the
Kolmogorov entropy, which is defined as the rate of
loss of information, the information of all colors is
actually mixed.
The description of the dynamics introduced in the
approach proposed is a priori irreducible to the notions
of the classical deterministic chaos theory with intro-
duction of a strange attractor in a multidimensional
phase space. Probably, as more adequate representa-
tions of such an evolution, one should consider the con-
cepts of the discrete chaotic dynamics, which have been
THEORETICAL FOUNDATIONSOF CHEMICALENGINEERING Vol. 34
311
recently discussed widely at international conferences
[31]. The proposed methodology itself can be regarded
as the phenomenological basis of the currently devel-
oping science of complexity, which deals with open
nonlinear dissipative systems of various essences--
actual natural objects. It is the science of complexity
that will be the basis for the reliable and confident "new
dialog with nature," about which Prigogine and
Stengers wrote [32].
ACKNOWLEDGMENTS
This work was supported by the INTAS Foundation,
project no. 97-30770.
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