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Thermodynamics properties of diatomic molecules with general molecular

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Article  in  Pramana · February 2018

DOI: 10.1007/s12043-017-1510-0

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Pramana – J. Phys. (2018) 90:22 © Indian Academy of Sciences
https://doi.org/10.1007/s12043-017-1510-0

Thermodynamics properties of diatomic molecules with general

molecular potential
AKPAN N IKOT1 ,∗ , E O CHUKWUOCHA1 , M C ONYEAJU1 , C A ONATE2 , B I ITA3
and M E UDOH1
1 Theoretical
Physics Group, Department of Physics, University of Port Harcourt, Port Harcourt, Nigeria
2 Department of Physical Sciences, Landmark University, Omu-Aran, Nigeria
3 Department of Chemistry, University of Calabar, Calabar, Nigeria
∗ Corresponding author. E-mail: [email protected]

MS received 23 August 2017; revised 15 September 2017; accepted 19 September 2017

Abstract. In this paper, the energy spectra of the general molecular potential are obtained using the asymptotic
iteration method within the framework of non-relativistic quantum mechanics.With the energy spectrum obtained,
the vibrational partition function is calculated in a closed form and is used to obtain an expression for other
thermodynamic functions such as vibrational mean energy U , vibrational mean free energy F, vibrational entropy
S and vibrational specific heat capacity C. These thermodynamic functions are studied for the electronic state X1 g+
of K 2 diatomic molecules.

Keywords. Asymptotic iteration method; diatomic molecules; general molecular potential; partition function.

PACS Nos 03.65.Ge; 03.65.Ca

1. Introduction used to calculate the thermodynamic properties of par-

tially ionised and dissociated gas of stellar atmosphere
The central point of studying the thermodynamics prop- [7]. Recently, Song et al [8] studied the thermodynamic
erties of a given system is to calculate its partition properties of sodium dimer with Rosen–Morse potential
function. The partition function, which is a function and Jia et al [9] investigated the thermodynamic prop-
of temperature, is usually regarded as the distribu- erties of lithium dimer with improved Manning–Rosen
tion function and if it is known, other thermodynamics potential model. In another development, Jia et al [10]
properties can be obtained from it. The vibrational obtained the partition function for improved Tietz oscil-
partition function of diatomic molecules for certain lators. Different mathematical techniques have been
potential models can easily be obtained by calculat- employed by many researchers in evaluating parti-
ing the rotation–vibrational energy levels of the sys- tion function such as Poisson summation fornula [11],
tem whose applications are widely used in statistical commulant expansion method [12], standard method
mechanics and molecular physics [1,2]. Strekalov [3] [13] and Wigner–Kirkwood formulation [14]. Moti-
obtained a closed form expression for the partition func- vated by the recent achievement in the determination
tion for Morse oscillators. The Morse oscillator has of the thermodynamic properties of some diatomic
been identified as the simplest and the most realis- molecules, we shall attempt to obtain the rotation–
tic oscillator model that has many applications in the vibrational energy spectrum for the general potential
description of vibrational state of diatomic molecules model using asymptotic iteration method (AIM) [15]
[4]. A simple analytic formula for the partition function and use the result to obtain a closed form expression
has been derived by Strekalov [5]. Maximum num- for the partition function which we shall use in calcu-
bers of vibrational and rotational states are needed to lating other thermodynamic properties of the diatomic
evaluate the partition function for the vibrational and molecules.
rotational states of diatomic molecules [6]. The result- The general molecular potential (GMP) model is
ing partition function had been reported to have been given by [16]
22 Page 2 of 9 Pramana – J. Phys. (2018) 90:22
 2
A − Be−α(r −re ) + q̃ C − De−α(r −re ) z(1 − z)ψ  (z) + (1 − z)ψ  (z)
V (r ) =  2 , (1) 1  2
1 − qe−α(r −re ) + γ1 z + γ2 z + γ3 ψ(z) = 0, (7)
z(1 − z)
where A, B, C, α are adjustable potential parameters, q̃, where
q are dimensionless parameters and re is the equilibrium
2μE J (J + 1)D0 2μD 2 q̃
bond length. To the best of our knowledge, no one has γ1 = − − 2 ,
reported the thermodynamic properties of GMP. h̄ 2 α 2 α2 h̄ α 2 q 2
4μE 2J (J + 1)D0 J (J + 1)D1
γ2 = − 2 + +
h̄ α 2 α 2 α2
2. Ro-vibrational energy spectrum 2μB 4μC D q̃
+ 2 + 2 ,
h̄ q α
2 2 h̄ α 2 q 2
The radial Schrödinger equation is defined as [17]
2μE J (J + 1)D0 J (J + 1)D1
  γ3 = 2 − −
d2 ψ(r ) 2μ J (J + 1)h̄ 2 h̄ α 2 α 2 α2
+ 2 E − V (r ) − ψ(r ) = 0, J (J + 1)D2 2μA 2μq̃C 2
dr 2 h̄ 2μr 2 − − − . (8)
(2) α2 h̄ 2 α 2 h̄ 2 α 2
A close inspection of eq. (7) shows that it has two sin-
where μ is the reduced mass, E is the ro-vibrational
gular points at z = 0 and z = 1. Thus, we can write the
energy, h̄ is the reduced Planck’s constant and J is
solution of eq. (7) as
the rotational quantum number. Substituting eq. (1) into
eq. (2) yields, ψ(z) = z μ (1 − z)σ f (z). (9)
d2 ψ(r ) 2μ Substituting eq. (9) into eq. (7), we obtain
+ 2
dr 2 h̄ (2μ + 2σ + 1)z − (1 + 2μ) 
  2 f  (z) = f (z)
A − Be−α(r −re ) + q̃ C − De−α(r −re ) z(1 − z)
 2 
× E−  2 σ + 2μσ + γ1 − γ3
1 − qe−α(r −re ) + f (z), (10)
 z(1 − z)
J (J + 1)h̄ 2 where
− ψ(r ) = 0. (3)
2μr 2 √
μ = i γ3 ,

In order to solve eq. (3), we invoke the following approx- 1 1

imation for the centrifugal term r −2 as [18] σ = + − (γ1 + γ2 + γ3 ). (11)
2 4
1 D1 D2 Now comparing eqs (10) and (6), we get the values of
≈ D0 + +  2 , (4)
r 2 1 − qe−α(r −re ) 1 − qe−α(r −re ) λ0 (z) and s0 (z) as follows:
(1 + 2μ + 2σ )z − (1 + 2μ)
where λ0 (z) =
  z(1 − z)
 2 
(3−αre )−2(3+αre )q + 3+3αre +α 2re2 q 2 σ + 2μσ + γ1 − γ3
D0 = , s0 (z) = . (12)
α 2 q 2re4 z(1 − z)
2(q − 1)2 (−3 + αre + 3q + 2αqre ) The corresponding ro-vibrational energy spectrum is
D1 = ,
α 2 q 2re4 calculated by means of the quantisation condition [15].
(q − 1)3 [3(q − 1) + (q + 1)αre ] With these, we obtain
 
D2 = . (5) 1 γ1 − γ3 + σ 2
α 2 q 2re4 s0 λ1 − s1 λ0 = 0 ⇒ μ0 = − ,
2 σ
In order to solve eq. (3) with the AIM, then we must s1 λ2 − s2 λ1 = 0 ⇒ μ1
transform eq. (3) into the form [15]  
1 γ1 − γ3 + σ 2 + 2σ + 1
=− ,
y  (x) = λ0 (x)y  (x) + s0 (x)y(x). (6) 2 σ +1
s2 λ3 − s3 λ2 = 0 ⇒ μ2
To do this, we make a coordinate transformation z =  
qe−α(r −re ) and this transform eq. (3) into the following 1 γ1 − γ3 + σ 2 + 4σ + 4
=− (13)
equation: 2 σ +2
Pramana – J. Phys. (2018) 90:22 Page 3 of 9 22
ν
max  νmax +1
and generally for arbitrary n, we have 1
  f (n) = [ f (0)− f (νmax + 1)] + f (x)dx.
γ3 − γ1 ν+σ ν=0
2 0
μn = − , (14)
2(ν + σ ) 2 (21)
where ν is the vibrational quantum number. Applying eq. (21) for the partition function of eq. (18),
Using eqs (8) and (11), we obtain the ro-vibrational we get
energy spectrum for the GMP as 
  1 −β  Q 2 − p1 p2   
2 − e−β Q 2 − p1 p3
2
h̄ 2 α 2 Q1 ν+σ 2 Z (β) = e
E nl = − + + Q2, (15) 2
 νmax   
2μ 2(ν + σ ) 2 −aβ− bβ2 −cβρ 2
where + e ρ dρ (22)
0
J(J + 1)(D1 + D2 )
Q1 = where
α  
2
 h̄ 2 α 2 Q1 νmax
2μ q̃ D p1 = , p2 = + ,
+ 2 + A + q̃C ,
2
2μ 2νmax 2
h̄ α 2 q 2  
J (J + 1)h̄ 2 Q1 (νmax + 1 + σ )
Q2 = (D0 + D1 + D2 ) p3 = + ,
2μ 2(νmax + 1 + σ ) 2
  h̄ 2 α 2 Q 21
+ A + q̃C 2 . (16) ρ = x + σ, a = − Q2,
4μ
h̄ 2 α 2 Q 21 h̄ 2 α 2
3. Partition function and thermodynamic b= , c= . (23)
8μ 4μ
properties
Evaluating the integral in eq. (22), we obtain the ro-
The total contribution of the bound state to the ro- vibrational partition function for the diatomic molecules
vibrational partition function of a diatomic molecule at with GMP model as
temperature T can be written as ⎡
1 ⎣ −β  Q 2 − p1 p2   
2 − e−β Q 2 − p1 p3
2
ν
max Z (β) = e
Z (β) = e−β E n,J , (17) 2
ν=0 ⎛
− 2bβ
 2ν e νmax
where β = (kB T )−1 with kB being the Boltzmann con- +e −cβρ 2 −aβ
bβ ⎝
max
√
stant and E ν,J is the rotation–vibrational energy of the bβ
νth bound state. Substituting eq. (16) into eq. (17) gives √ √  ⎞⎤
bβ
 2  2 bπβerf νmax √
ν
− 2 π ⎠⎦ ,
2 2
max
−β Q 2 − h̄ 2μα 2(ν+σ
Q1
) + ν+σ
2 + √ (24)
Z (β) = e , (18) bβ
ν=0
where erfi(x) is the imaginary error function defined as
where
[8,9]
 1    x
νmax = Q1 − 1 + 1 − 4(γ1 + γ2 + γ3 ) . 2 2
2 erfi(x) = −ierf(i x) = √ et dt (25)
(19) π 0

In order to evaluate partition function, we write the Pois- and erf(x) denotes the error function which is a special
son summation formula as [3,5,11], function of the sigmoid shape [8,9]. In Maple software
the imaginary error function is given as erfi(x) and can
ν
max
1 be used in many numerical calculations.
f (n) = [ f (0) − f (νmax + 1)] We have plotted in figure 1a, the exact and semiclas-
2
ν=0 sical partition functions as a function of temperature.
 ∞  νmax +1
Also, we have plotted the exact, semiclassical partition
+ f (x)e−i2π mx dx. (20) including zero temperature in figure 1b. As shown in fig-
m=−∞ 0 ure 1a, the semiclassical partition function is very close
However, for the lowest order approximation, the to the exact partition function. It deviates from exact par-
Poisson summation formula becomes [3,5,11] tition function as the temperature increases. Similarly,
22 Page 4 of 9 Pramana – J. Phys. (2018) 90:22

as shown in figure 1b the semiclassical partition func-

tion deviates from the exact partition function and it is
approximately the same at zero temperature.
With the help of the vibrational partition function of
eq. (24), we can determine the thermodynamic proper-
ties for the potential model as follows:

(1) The vibrational mean energy U

∂ n Z (β)
U (β) = −
∂β
⎛ ⎛
− 2βb
1  2ν e νmax
= −⎝ e −cρ
βb ⎝
2 β−aβ max
√
2 βb
√ √  ⎞
βb
2 βberf νmax √
+ √ − 2 π⎠
βb
⎞−1
1    
⎠
e−β Q 2 − p1 p2
− e−β Q 2 − p1 p3
2 2
+
2
× [1 + 2 ] , (26)

where
⎛
− 2βb
1 2  −cρ 2 β−aβ  2ν e νmax
βb ⎝
max
1 = − cρ + a e √
2 βb
√ √  ⎞
βb
2 πβberf νmax √
+ √ − 2 π⎠
βb
⎛
− 2βb
1 −cρ 2 β−aβ  ⎝ 2νmax e νmax
+ e βb √
4 βb
√ √  ⎞
βb
2 πβberf νmax √
+ √ − 2 π ⎠ B, (27)
βb
⎛
− 2βb
1 −cρ 2 β−aβ  ⎝ −νmax e νmax b
2 = e βb 3
2 (bβ) 2
3√
√  √ √ 
βb βb
b 2 βπerf νmax βberf νmax
− + √
Figure 1. (a) Plot of the exact partition function (eq. (18)) 3
(bβ) 2 βb
and the semiclassical partition function (eq. (22)) as a function ⎞
of β at νmax = 25, (b) plot of the exact partition function (eq. √ 1 −β  Q 2 − p1 p2   
−2 π ⎠ + 2 − e−β Q 2 − p1 p3
2
(18)) and the semiclassical partition function (eq. (22)) as e .
a function of β at zero temperature and at νmax = 25 and 2
(c) vibrational partition function Z as a function of β for
different νmax . (28)
Pramana – J. Phys. (2018) 90:22 Page 5 of 9 22

(2) Vibrational mean free energy F

⎛ ⎡
1 1 ⎝ 1 ⎣ −β  Q 2 − p1 p2   
2 − e−β Q 2 − p1 p3
2
F = − n Z (β) = − n e
β β 2
⎛ √ √  ⎞⎤ ⎞
− 2bβ bβ
 2νmax e ν max 2 bπβerf νmax √
+ e−cβρ −aβ bβ ⎝ − 2 π ⎠⎦ ⎠ .
2
√ + √ (29)
bβ bβ

(3) Vibrational specific heat capacity C

 
∂U 2 ∂U (β) 21 ϒ
C= = −kβ = −kβ (30)
∂T ∂β  
where
⎛ ⎛ √ √  ⎞ ⎞2
− 2βb βb
1  2νmax e ν max 2 πβberf νmax √ 1   1  
 = ⎝ e−βcρ −aβ bβ ⎝ − 2 π ⎠ + e−β Q 2 − p1 p2 − e−β Q 2 − p1 p3 ⎠ ,
2 2 2
√ + √
2 βb βb 2 2
(31)
⎛ ⎛ βb √ √  ⎞ ⎞
− βb
1  2νmax e 2
νmax 2 π bβerf νmax √ 1   1  
 = ⎝ e−βcρ −aβ βb ⎝ − 2 π ⎠ + e−β Q 2 − p1 p2 − e−β Q 2 − p1 p2 ⎠
2 2 2
√ + √
2 βb βb 2 2
⎛  βb √ √   ⎞2
− 2
  −βcρ 2 −aβ √ 2νmax e ν 2 π bβerf βb
νmax √
⎜ 2 −cρ − a e βb + −2 π
1 2 max
√ √ ⎟
⎜ βb βb ⎟
⎜  √   ⎟
⎜ − 2
βb √ βb ⎟
⎜ 1 e−βcρ 2 −aβ 2νmax e νmax 2 π bβerf νmax √ ⎟
⎜+4 √ √ + √ −2 π b ⎟
⎜ βb βb βb ⎟
⎜ ⎛   ⎞ ⎟
⎜ βb βb √ √ √ √ ⎟
−⎜ − 2
−2be √νmax
− 2
νmax be νmax π bβerf βb
b πβbβerf βb
⎟ , (32)
⎜ √ ⎜ − + √
νmax
−
νmax
⎟ ⎟
⎜ 1 −βcρ 2 −aβ ⎜ ν βb 3
β b 3 ⎟⎟
⎜+2e βb ⎜ max bβ (bβ) 2 (βb) 2 ⎟⎟
⎜ ⎝ − 2 ⎠⎟
⎜ νmax ⎟
⎜ + 2be √ ⎟
⎜ νmax βb ⎟
⎝ ⎠
   
+ 21 e−β Q 2 − p1 p22
− 21 e−β Q 2 − p1 p22

⎛ ⎛ √ √  ⎞⎞
− 2bβ bβ
1 2  2νmax e ν max 2 π bβerf νmax √
ϒ = ⎝ −cρ 2 − a e−βcρ −aβ bβ ⎝ − 2 π ⎠⎠
2
√ + √
2 bβ bβ

 −βcρ 2 −aβ ⎛ ⎞
√ √
 − 2bβ bβ
1 −cρ − a e
2
2ν e ν max 2 π bβerf ν √
+ √ ⎝ max √ + √
max
− 2 π⎠ b
2 bβ bβ bβ
√ √  √ √ 
bβ − 2bβ bβ
bβerf νmax 2be νmax π bβerf νmax b   
+ −cρ 2 − a e−βcρ −aβ bβ
2
+ √ + √ −
β b νmax bβ (bβ) 2
3

⎛ bβ bβ ⎞ ⎛
− 2 − 2 − 2bβ
−2be ν max ν be ν max 1 e −βcρ 2 −aβ
2ν e νmax
×⎝ √ ⎠− ⎝
max max
− 3
√
bβ (bβ) 2 8 (bβ) 23 bβ
√ √  ⎞ ⎛
bβ − 2bβ − 2bβ
2 bπβerf νmax √ 1 e −βcρ 2 −aβ −2be νmax 2ν be νmax
− 2 π ⎠ b2 + ⎝ max
+ √ √ √ −
bβ 2 bβ νmax bβ (bβ) 2
3
22 Page 6 of 9 Pramana – J. Phys. (2018) 90:22
√ √  √ √  ⎞
bβ − 2bβ bβ
bπβerf νmax 2be νmax bπβerf νmax b √
+ √ + √ − − 2 π⎠ b
β b νmax bβ 3
(bβ) 2
⎛ bβ bβ √ √  bβ
− 2
⎞
− 2 bβ − 2
bβerf νmax
2b2 e √νmax 2b2 e νmax 3 νmaxb2 e νmax
 ⎜ νmax bβ
+ − 1
3√ + ⎟
1 ⎜ 3 3 2 2 5
⎟
+ e−βcρ −aβ bβ ⎜ νmax (bβ) 2 β 2 bβ
2
(bβ) 2
√ √  √ √  ⎟
⎝
bβ bβ bβ
2 bπerf νmax bβ
b − 2 5 − 2 5 − 2 bβ
bβπerf νmax b2 ⎠
be νmax 2b 2 e √νmax 2b 2 e νmax
− √ 3 + 1 − ν3 − 3 + 3
2 5
β(bβ) 2 βνmax (bβ) 2 max bβ νmax (bβ) 2 (bβ) 2
1 2   1 2  
Q 2 e−β Q 2 − p1 p2 − p1 p32 − Q 2 e−β Q 2 − p1 p3 .
2 2
+ p1 p22 − (33)
2 2
⎛ bβ
−
(4) Vibrational entropy S 1 e−βcρ −aβ
2 2
⎝ 2νmax e νmax
+ √ √
4 bβ bβ
∂ √  ⎞
S = k n Z (β) − kβ n Z (β) √ bβ
∂β 2 π bβerf νmax √
kβ + √ − 2 π ⎠ b, (35)
= k n Z (β) − (1 + 2 ) , (34) bβ
⎛
Z (β) − 2bβ
1 −βcρ 2 −aβ  −ν be νmax
bβ ⎝
max
2 = e 3
where 2 (bβ) 2
√ √  3√
√ ⎞
bβ bβ
 π berf νmax b 2 πβerf νmax
1 
+ √ − ⎠
−cρ 2 − a e−βcρ −aβ bβ
2
1 =
β b
3
2 √  (bβ) 2
⎛ √ ⎞
− 2bβ bβ
2νmax e ν 2 π bβerf νmax √ 1 2  
+ p1 p22 − Q 2 e−β Q 2 − p1 p2
max 2
×⎝ √ + √ − 2 π⎠ 2
bβ bβ
1 2  
− p1 p32 − Q 2 e−β Q 2 − p1 p3 .
2
(36)
2

Figure 2. Vibrational partition function Z as a function of Figure 3. Vibrational mean energy U as a function of β for
νmax for different β. different νmax .
Pramana – J. Phys. (2018) 90:22 Page 7 of 9 22

Figure 6. Vibrational entropy as a function of νmax for dif-

ferent β.
Figure 4. Vibrational mean energy U as a function of νmax
for different β.

Figure 5. Ro-vibrational entropy S as a function of β for

different νmax .
Figure 7. Vibrational specific heat capacity as a function of
β for different νmax .

4. Discussions

In this paper, we consider electronic state of the potas- The experimental values of X1 g+ states of potas-
sium dimer K 2 (X1 g+ ) molecules using the energy sium (K 2 ) dimer are taken from ref. [19]: De =
eigenvalues of eq. (15). We take into account the GMP 4400.00 cm−1 , re = 3.9244 A, α = 0.0562×103 cm−1
with the following potential parameters as [16] and μ = 19.4800 U. Now using these experimental data
as our input, we plot the vibrational partition function for
A + q̃C 2 = De ,
the X1 g+ states of K 2 for various upper bound vibration
(B + 2q̃C D) = 2De , quantum number νmax = 25, 50 and 75 and temper-
q = − exp(−αre ) . (37) ature β = 0.005, 0.008 and 0.01 in figures 1 and 2
22 Page 8 of 9 Pramana – J. Phys. (2018) 90:22

Figure 8. Vibrational specific heat capacity as a function of Figure 10. Vibrational free energy as a function of νmax for
νmax for different β. different β.

β and upper bound vibration quantum number νmax in

figures 5 and 6 respectively. It is shown that the entropy
S monotonically increases as β and νmax increase for
the potassium dimer. Figures 7 and 8 show the plot of
the vibrational specific heat capacity C of potassium
dimer. In figure 7 the specific heat capacity C decreases
with increase in temperature. However, in figure 8, the
specific heat capacity first increases to maximum values
and converge as νmax is increased. The plot of the mean
free energy F is shown in figures 9 and 10. As shown
in figure 9 the mean free energy F decreases monoton-
ically with increasing νmax while F increases with β as
shown in figure 10.

5. Conclusions

In this work, we solved the Schrödinger equation with

GMP within the framework of asymptotic iteration
method and obtained the energy spectra in a closed form.
Figure 9. Vibrational free energy F as a function of β for We calculated the vibrational partition function Z in a
different νmax .
closed form and used it to study the thermodynamic
properties of vibrational mean energy U , vibrational
entropy S, vibrational mean free energy F and vibra-
respectively. It is observed that the partition function Z tional specific heat capacity C. We have plotted the
monotonically increases as β and νmax increase for the behaviour of the thermodynamic functions as a func-
potassium dimer. We show in figures 3 and 4 the plot tion of temperature β and the upper bound vibration
of the vibrational mean energy for various values of β quantum number νmax for the electronic state X1 g+ of
and νmax . It shows that the mean energy U decreases potassium dimer. Finally, the improved Rosen–Morse
monotonically with increasing values of β and νmax . [20] and Manning–Rosen potentials [21,22] are all spe-
We plotted the entropy S as a function of temperature cial cases of general molecular potential [16] and this
Pramana – J. Phys. (2018) 90:22 Page 9 of 9 22

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system [23] and in non-central potential model [24]. II, Infared and Raman spectra of polyatomic molecules
(Van Nostrand, New York, 1945)
[13] A N Ikot, B C Lutfuoglu, M I Ngwueke, M E Udoh, S
Zare and H Hassanabadi, Eur. Phys. J. Plus 131, 419
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