+
(1)
Eq. (1) denotes the situation where a free adsorption site
A
f
and a free gas particle A
g
stochastically and reversibly
change into an adsorbate particle A
a
with an adsorption
The Poissonian Nature of
AdsorptionDesorption Processes
Olga M. Jaki, Zoran S. Jaki, Senior Member, IEEE and Danijela V. Randjelovi, Member,
IEEE, eljko D. upi, Ljiljana Z. KolarAni
T
20th Telecommunications forum TELFOR 2012 Serbia, Belgrade, November 2022, 2012.
9781467329842/12/$31.00 2012 IEEE 206
rate constant k
a
'', while the desorption rate constant is k
d
.
The corresponding kinetic equation is
( ) ( )
0
''
''
a
a g f d a
a a a d a
dN
k N N k N
dt
k N N M N k N
=
=
(2)
N denotes numbers, indices denote reactants, N
0
is the
overall number of particles in the system and M is the
number of adsorption centers on the surface. In case N
0
greatly exceeds M (valid for pressures and surfaces in the
majority of engineering situations [12]), even if the whole
surface is populated, N
0
does not decrease significantly
and this expression transforms into a linear first order
differential equation
( )
( )
0
0
''
, ''
a
a a d a
a a d a a a
dN
k N M N k N
dt
k M N k N k k N
= =
(3)
All further analysis is valid for the latter model.
III. THE STOCHASTIC NATURE OF AN ADSORPTION
DESORPTION PROCESS
A. The probability generating function
Generating functions connect the discrete and the
continous mathematical approaches to the problems. They
transform functional problems into problems about
sequences. Here we give the definition of the probability
generating function (PGF) and its properties used through
out our stochastic analysis to determine the probability
distribution of the number of adsorbed particles.
If we denote the number of adsorbed particles on the
solid surface with x and the probability that in time instant
t will be x adsorbed particles on that surface with P
x
(t), the
monovariate PGF is
( ) ( ) ( )
( ) ( )
1
1
0 0
1
1 0
0
,
1
x x
x x
x x
x
x
x
F s t P t s P t s
s
P t s P t
= =
+
+
=
= =
= +
_ _
_
(4)
The first derivative of this PGF is
( )
( ) ( ) ( )
( ) ( ) ( )
1 2
1
0 0
1 0
0
,
1
1 0 , 1
x x
x x
x x
x
x
x
F s t
xP t s x P t s
s
x P t s P t s
= =
+
=
= =
= + +
_ _
_
(5)
The second derivative is
( )
( ) ( )
( ) ( ) ( )
( ) ( ) ( )
2
2
2
0
3
1
0
1
1 0
0
,
1
1 2 1
1 0
x
x
x
x
x
x
x
x
x
F s t
x x P t s
s
x x P t s s
x xP t s P t
+
=
=
= + +
_
_
_
(6)
The derivatives of the PGF with respect to s satisfy
( )
( ) ( )
1
,
E 1 1
i
i
s
F s t
x x x i
s
=
( = +
(7)
Based on this expression, all moments can be
straightforwardly found [13].
B. The stochastic analysis
For the adsorptiondesorption system under
consideration we assumed the following: the surface is
nonporous, homogeneous (all binding sites are equal);
initially all binding sites are free. Gas is ideal, all particles
alike, noninteracting with each other, forming only
monolayers on the surface.
The state space for the system comprises M + 1 possible
states (the number of adsorbed molecules is N
a
, we will
denote it here with x for the sake of compactness of long
expressions; N
a
= x may be 0, 1, 2, , M). The time span
for our system observations t is small enough, so that
only transitions between the neighboring states may occur.
The system can reach the state with x adsorbed molecules
in three ways:
the system was in a state with x 1 adsorbed
molecules and then one more is adsorbed;
the system was in a state with x + 1 adsorbed
molecules and then one is desorbed;
the system was in a state with x adsorbed molecules
and no transitions occurred.
The transition probabilities between these states are
( ) ( )
( ) ( )
( ) ( ) ( ) ( )
1
1
1
a a
d d
a a d d
P x x k x t o t
P x k x t o t
P x x k x k x t o t
= +
+ = +
= + +
(8)
where o(t) is the Landau order symbol meaning that it
vanishes with a higher order than its argument t. The first
transition is a consequence of adsorption and x
a
is the
number of free adsorption centers at that particular
moment, i.e. x
a
= M (x1). The second transition is a
consequence of desorption and x
d
is the number of
adsorbed molecules for that case, x
d
= (x + 1). The only
possible situation left is when no transitions occur, and
then x
a
= Mx and x
d
= x. The probability that the system
will be in a state with x = N
a
adsorbed molecules, t time
units after t is
( ) ( ) ( )
( ) ( ) ( ) ( )
1
1
1
1
x x
x x
P t t P t P x x
P t P x x P t P x x
+
+ =
+ + +
(9)
Hence, with all that in mind, eq. (8) and (9) give
( ) ( ) ( ) ( ) ( )
( ) ( ) ( )
( ) ( ) ( ) ( )
( )
1
1
1
1
1
x x a
x d
x a d
P t t P t k M x t o t
P t k x t o t
P t k M x k x t o t
+
(
+ = +
( + + +
(
+ + +
(10)
After regrouping and taking the limit when t 0 we
get the Kolmogorov differential equation for probability
function
( )
( ) ( ) ( ) ( ) ( )
( ) ( ) ( )
1 1
d
1 1
d
x
x a x d
x a d
P t
P t k M x P t k x
t
P t k M x k x
+
= + +
+
(11)
We now multiply the expression (11) by an infinite
power series of s, and sum over x. We group the members
so that one can recognize the probability generating
function of the P
x
(t) and its derivatives.
207
( ) ( )
( ) ( ) ( ) ( )
( ) ( ) ( )
1
1
0 0
2 2
1 1
0 0
1
0 0
1 1
x x
x a x
x x
x x
a x d x
x x
x x
a x a d x
x x
d
s P t k Ms P t s
dt
k s x P t s k x P t s
k M P t s k k s xP t s
= =
+
= =
= =
 
=

\ .
+ +
+
_ _
_ _
_ _
(12)
Since all probabilities beyond physical limits (involving
x out of the range 0, M) are zero, by the use of
definitions (4), (5) and (6), eq. (12) becomes
( )
( )
( ) ( )
( ) ( )
( )
2
, , ,
,
,
,
a a d
a a d
F s t F s t F s t
k MsF s t k s k
t s s
F s t
k MF s t k k s
s
= +
(13)
Using this method, eq. (11), difference differential
equation over probability, is transformed at the end into
the partial differential equation over PGF generating
function
( )
( )
( )
( )
( ) ( )
2
, ,
1 ,
d a d a
a
F s t F s t
k k k s k s
t s
k M s F s t
= +
+
(14)
The initial condition corresponding to N
a
(0)=0 is
F(s,0)=1 and the solution to this linear partial differential
equation is
( )
( )
( )
( )
0
,
1
a d
M
k k t a x a d
x
a d a d x
F s t
k s k s k
P t s e
k k k k
+
=
=
( +
= +
(
+ +
(
_
(15)
In order to extract the probability distribution function
we regroup the binome members and get
( )
( )
( )
( )
1
,
a d
a d
M
k k t
k k t
a
a d
a d a d
k e
k e k
F s t s
k k k k
+
+
(
+
(
= +
(
+ +
(
(16)
Written in a form of series, this expression is
( )
( )
( )
( )
0
,
1
a d
a d
x
k k t M x
k k t
M
a
a d
a d a d x
F s t
sk e
M k e k
x k k k k
+
+
=
=
 
 
+   



 + +
\ .
 \ .
\ .
_
(17)
The exact probability distribution function is then
( )
( )
( )
( )
1
a d
a d
x
x
k k t M x
k k t
a
a d
a d a d
P t
k e
M k e k
x k k k k
+
+
=
 
 
+   



 + +
\ .
 \ .
\ .
(18)
The sum of all probabilities over all possible numbers of
adsorbed molecules must be 1, which is satisfied.
IV. THE PROBABILITY DISTRIBUTION OF A POISSONIAN
PROCESS
The Poisson distribution stems from Bernoullie's (also
called binomial) distribution. In a total of N outcomes of a
stochastic variable that can have either one outcome with a
probability p or the opposite outcome with a probability
q = 1 p, the probability that that stochastic event occurs
exactly n times is
( ) ( ) 1
n
N
N
p n p p N n
n
 
=

\ .
(19)
Fig. 1 shows this distribution for various pairs of (N, p).
Fig. 1. Binomial distribution for different pairs of (N, p)
In case there are some constraints that force the
probability to proportionally decrease with an increase of
N, and that is the case with all examples from the
introduction (the number of servers, service centers or
places in a queue is finite), all distributions converge to the
same one like that shown in Fig. 2. That distribution is
Poissonian and the mathematical expression stems from
( )
( ) ( ) ( ) ( )
( ) ( )
1 2 1 1
!
1 2 1
1 1 1 1 1
!
N n
n
N
n N n
N N N N n p p
p n
n
n
pN p
N N N
n
+
=
    
  
\ .\ . \ .
=
(20)
For a constant product of N and p, equal to , we get
( )
1
1
1
1
!
1
N
n n
N
n
i
i N
p n
N n
N
=
 

  \ .
=

\ .
 

\ .
(21)
For a very large N it holds that
( ) lim
!
n
N
N
p n e
n
= (22)
V. DISCUSSION
If we adopt the notation from the previous section and
put
( )
( )
1
a d
k k t
a
a d
k e
p
k k
+
=
+
(23)
and check
( )
( )
( ) 1
1
a d
a d
k k t
k k t
a
a d
a d a d
k e
k e k
k k k k
+
+
+
=
+ +
(24)
we see that the true probability distribution of an
208
adsorptiondesorption process, eq. (18), is actually
binomial. For a large M the process can be treated as
Poissonian with the parameter
( )
( )
1
a d
k k t
a
a d
k M e
Mp
k k
= =
+
(25)
Fig. 2. Binomial distribution for different pairs of (N, p)
in case their product is constant, =50.
So, if M is large, this means that the number of
adsorption centers on the surface is large. Thus according
to the first assumption we made, this whole model (eq. 3)
is valid if that number is greatly exceeded by the overall
number of particles in the system. Practically, that means
that the surface is large and surrounding gas is under high
pressure. But high pressures lead to a situation where
multilayers of adsorbed particles/molecules may occur on
the surface and even the first two equations cease to be
valid (the model is for monolayer adsorption).
From a practical point of view, the pressure is not the
designers' dilemma. The question is not "What is the
minimal pressure that provides that eq. (3) is still valid and
what is the maximum pressure beyond which eqs. (1) and
(2) do not hold any more". Pressure is the subject of
unpredictable situation and the question is "With the given
set of determined physical parameters, how to design a
sensor area (that affects the adsorption rate constant k
a
and
the number of adsorption sites M) that meets the
predictions and the performances derived with the
treatment of an adsorptiondesorption process as a first
order chemical reaction with a Poissonian probability
distribution function, or (in the case M is set), should I do
the research analysis and optimizations all over again
presuming second order chemical reaction or the binomial
probability distribution?".
From Fig. 2, it is enough for N to be 20 times greater
than in order to be reasonable to treat the process as
Poissonian, but the augmentation of M does not
necessarily mean that p will be proportionally decreased
and preserved. The physical parameters of a target gas
species for which we design the sensor affect adsorption
kinetics through the sorption rate constants [12] and do not
alter with scaling. The physical parameters of a material
for sensor surface are also fixed.
VI. CONCLUSION
It is proven in this work that the exact probability
distribution function of an adsorptiondesorption process is
binomial. The conditions for the assumption of a
Poissonian distribution function may be met in a praxis,
but should be checked for each particular situation.
ACKNOWLEDGMENT
To Diana StojanoviWongkaren for discussions.
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THE POISSONIAN NATURE OF
ADSORPTIONDESORPTION PROCESSES
Olga M. Jaki, Zoran S. Jaki, Senior Member,
IEEE and Danijela V. Randjelovi, Member, IEEE,
eljko D. upi, Ljiljana Z. KolarAni
209
Steering Committee / Upravni odbor
Prof. Dr ore Paunovi, Chair/Predsednik, TS/DT, ETF,
Belgrade, Serbia
Prof. Dr Branko Kovaevi, Dean/Dekan, ETF, Belgrade, Serbia
Prof. Dr Aleksandar Nekovi, Chair/Predsednik, TPC, ETF,
Belgrade, Serbia
Prof. Dr Ljiljana Mili, Chair/Predsednik, Org. Committee, IMP,
ETF, Belgrade, Serbia
Prof. Dr Irini Reljin, Vice Chair/Potpredsednik, TPC, ETF,
Belgrade, Serbia
Prof. Dr Nataa Nekovi, Chair IEEE S&M Section, ETF,
Belgrade, Serbia
Technical Program Committee (TPC) / Programski odbor
Prof. Dr Aleksandar Nekovi, Chair/Predsednik, ETF, Belgrade,
Serbia
Prof. Dr Irini Reljin, Vice Chair/Potpredsednik, ETF, Belgrade,
Serbia
Prof. Dr Nataa Gospi, SF, Belgrade, Serbia
Prof. Dr Vlado Deli, FTN, Novi Sad, Serbia
Prof. Dr Duan Draji, ETF, Belgrade, Serbia
Prof. Dr Miroslav Duki, ETF, Belgrade, Serbia
Academician Prof. Dr Antonije orevi, SANU, ETF, Belgrade,
Serbia
Prof. Dr Jovan orevi, ETF, Belgrade, Serbia
Mr Nenad Krajnovi, ETF, Belgrade, Serbia
Prof. Dr Miroslav Lutovac, Singidunum University, Belgrade,
Serbia
Prof. Dr Miomir Miji, ETF, Belgrade, Serbia
Prof. Dr Ljiljana Mili, IMP, ETF, Belgrade, Serbia
Prof. Dr Nataa Nekovi, ETF, Belgrade, Serbia
Prof. Dr Zorica Nikoli, EF, Ni, Serbia
Prof. Dr ore Paunovi, ETF, Belgrade, Serbia
Prof. Dr Predrag Pejovi, ETF, Belgrade, Serbia
Prof. Dr Vladimir Petrovi, ETF Belgrade, Serbia
Prof. Dr Grozdan Petrovi, ETF, Belgrade, Serbia
Prof. Dr Miodrag Popovi, ETF, Belgrade, Serbia
Prof. Dr Jelica Proti, ETF, Belgrade, Serbia
Prof. Dr Branimir Reljin, ETF, Belgrade, Serbia
Prof. Dr Abdalla Abdulgader, Univ., Libya
Prof. Dr ura Budimir, Univ. Westminster, London, UK
As. Prof. Dr Zoran Veljovi, ETF, Podgorica, Montenegro
Prof. Dr Branka Vueti, Univ.Sidnej, Australia
Prof. Dr Octavian Fratu, Univ. Politehnica, Bucharest, Romania
Prof. Dr Liljana Gavrilovska, UKIM, Skopje, Makedonia
Dr Alexander Gelman, NETovarions group, IEEE ComSoc,USA
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Prof. Dr Simona Halunga, Univ. Politehnica, Bucharest, Romania
Prof. Dr Toni Janevski, UKIM, Skopje, Makedonia
Prof. Dr Venceslav Kafediski, UKIM, Skopje, Makedonia
Prof. Dr Ivo Kosti, ETF, Podgorica, Montenegro
Dr George Koutitas, Internat. Hellenic Univeristy, Thessaloniki,
Greece
Prof. Dr Rolf Kraemer, IHP Microelectronics, Frankfurt, Germany
Dr Milo Krsti, IHP Microelectronics, Frankfurt, Germany
Prof. Dr Milica Pejanoviurii, ETF, Podgorica, Montenegro
Prof. Dr Igor Radusinovi, ETF, Podgorica, Montenegro
Prof. Dr Zbynek Raida, Dept. Radio El., Brno, Czech Republic
Prof. Dr Kurt Richter, Tech. Univ., Graz, Austria
Prof. Dr Sherif Welsen Shaker, KuangChi Institute of
Adv.Technology, Shenzhen, China
Prof. Dr Hannes Topfer, Tech. Univ., Ilmenau, Germany
Prof. Dr. Ion Tutanescu, Fac. ECC, Univ. of Pitesti, Romania
As. Prof. Dr Matej Zajc, Univ. Ljubljana, Slovenia
Scientific Committee / Nauni odbor
Prof. Dr Ljiljana Mili, IMP, ETF, Belgrade, Serbia
Prof. Dr Duan Draji, ETF, Belgrade, Serbia
Filip Bankovi, Telekom Serbia
As. Prof. Dr Milan Bjelica, ETF Belgrade, Serbia
Dr Dragan Bogojevi, TS, Belgrade, Serbia
As. Prof. Dr Dragan Boji, ETF Belgrade, Serbia
Prof. Dr Zoran Bojkovi, SF, Belgrade, Serbia
Prof. Dr Branka Vueti, Univ.Sidnej, Australija
Prof. Dr ura Budimir, Univ. Westminster, London, UK
As. Prof. Dr Zoran Veljovi, ETF, Podgorica, Montenegro
Dr Alexander Gelman,IEEE ComSoc,USA
Prof. Dr Nataa Gospi, SF, Belgrade, Serbia
Prof. Dr Vlado Deli, FTN, Novi Sad, Serbia
Dr Dejan Draji, Iritel, ETF, Belgrade, Serbia
Prof. Dr Miroslav Duki, ETF, Belgrade, Serbia
Prof. Dr Jovan orevi, ETF, Belgrade, Serbia
Academician Prof. Dr Antonije orevi, ETF, SANU, Belgrade,
Serbia
Ljiljana orevi, Telekom Serbia
Prof. Dr Goran orevi, EF Ni, Serbia
Milivoje uni, TS, Belgrade, Serbia
Prof. Dr Octavian Fratu, Univ. Politehnica, Bucharest, Romania
Prof. Dr Liljana Gavrilovska, UKIM, Skopje, Makedonia
Dr Apostolos Georgiadis, CTTC, Barcelona, Spain
Prof. Dr Simona Halunga, Univ. Politehnica, Bucharest, Romania
As. Prof. Dr Predrag Ivani, ETF Belgrade, Serbia
Prof. Dr Toni Janevski, UKIM, Skopje, Makedonia
As. Prof. Dr Milan Jankovi, RATEL, Serbia
Mr Mihailo Jovanovi, PTT Serbia
Prof. Dr Venceslav Kafediski, UKIM, Skopje, Makedonia
Prof. Dr Vladimir Kati, IEEE, FTN, Novi Sad, Serbia
Dragan M. Kovaevi, IRITEL, Belgrade, Serbia
Dr Milan . Kovaevi, SAGA, Belgrade, Serbia
Prof. Dr Ivo Kosti, ETF, Podgorica, Montenegro
Dr George Koutitas, Internat. Hellenic Univeristy, Thessaloniki,
Greece
Prof. Dr Rolf Kraemer, IHP Microelectronics, Frankfurt, Germany
Dr Milo Krsti, IHP Microelectronics, Frankfurt, Germany
Prof. Dr Husnija Kurtovi, ETF Belgrade, Serbia
Prof. Dr Borivoj Lazi, ETF, Belgrade, Serbia
As. Prof. Dr. Josip Lorincz, FESB, Univ. of Split, Croatia
Prof. Dr Miroslav Lutovac, SINGIDUNUM University, Belgrade,
Serbia
Prof.dr Veljko Milutinovi, ETF Belgrade, Serbia
Prof. Dr Miomir Miji, ETF, Belgrade, Serbia
Prof. Dr Bratislav Milovanovi, EF, Ni, Serbia
Prof. Dr Vladimir Miloevi, FTN, Novi Sad, Serbia
Ivan Nador, Telekommunications Society, Belgrade
Zorica Nestorovi, Telekom Serbia
Prof. Dr Aleksandar Nekovi, ETF, Belgrade, Serbia
Prof. Dr Nataa Nekovi, ETF, Belgrade, Serbia
Prof. Dr Boko Nikoli, ETF Belgrade, Serbia
Prof. Dr Zorica Nikoli, EF, Ni, Serbia
Prof. Dr ore Paunovi, ETF, Belgrade, Serbia
Prof. Dr Milica Pejanoviurii, ETF, Podgorica, Montenegro
Prof. Dr Vladimir Petrovi, ETF Belgrade, Serbia
Prof. Dr Grozdan Petrovi, ETF, Belgrade, Serbia
Dr Predrag Petrovi, IRITEL, Belgrade, Serbia
Academician Prof. Dr Dejan Popovi, ETF, SANU, Belgrade,
Serbia
Prof. Dr Mirjana Popovi, ETF, Belgrade, Serbia
Prof. Dr Miodrag Popovi, ETF, Belgrade, Serbia
As. Prof. Dr Milka Potrebi, ETF, Belgrade, Serbia
Prof. Dr Jelica Proti, ETF, Belgrade, Serbia
Prof. Dr Jovan Radunovi, RATEL, ETF, Belgrade, Serbia
Prof. Dr Igor Radusinovi, ETF, Podgorica, Montenegro
Prof. Dr Zbynek Raida, Dept. Radio El., Brno, Czech Republic
Prof. Dr Branimir Reljin, ETF, Belgrade, Serbia
Prof. Dr Irini Reljin, ETF, Belgrade, Serbia
Prof. Dr Kurt Richter, Tech. Univ., Graz, Austria
As. Prof. Dr Mirjana Simi, ETF, Belgrade, Serbia
Momilo Simi, Telecommunications Society, Belgrade
As. Prof. Dr Lazar Saranovac, ETF, Belgrade, Serbia
Prof. Dr Sherif Welsen Shaker, KuangChi Institute of
Adv.Technology, Shenzhen, China
Milan Simi, Telekom Serbia
Prof. Dr Nenad Simi, ETF, Belgrade, Serbia
Prof. Dr Aleksandra Smiljani, ETF, Belgrade, Serbia
As. Prof. Dr Mirjana Stojanovi, SF, ETF, Belgrade, Serbia
Prof. Dr Zlatan Stojkovi, ETF, Belgrade, Serbia
Mr Ivan Teleki, TS, Novi Sad, Serbia
Prof. Dr Miodrag Temerinac, FTN, Novi Sad, Serbia
Prof. Dr Hannes Topfer, Tech. Univ., Ilmenau, Germany
Prof. Dr Dejan Toi, ETF, Belgrade, Serbia
Prof. Dr eljen Trpovski, FTN Novi Sad, Serbia
As. Prof. Dr Matej Zajc, Univ. Ljubljana, Slovenia