Journal of Magnetism and Magnetic Materials 402 (2016) 101–104

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Journal of Magnetism and Magnetic Materials

journal homepage: www.elsevier.com/locate/jmmm

Pair approximation method for spin-1 Heisenberg system

Murat Mert a, Ahmet Kılıç b, Gülistan Mert a,n
a
Department of Physics, Selcuk University, 42075 Konya, Turkey
b
Department of Physics, Ankara University, 06100 Ankara, Turkey

art ic l e i nf o a b s t r a c t

Article history: Spin-1 Heisenberg system on simple cubic lattice is considered in the pair approximation method as-
Received 3 October 2015 suming that the second-nearest-neighbor exchange interaction parameter has a negative value. The
Received in revised form system is described in presence of an external magnetic field. The effects of the negative single-ion
3 November 2015
anisotropy and the negative second-nearest-neighbor exchange interaction on magnetization, internal
Accepted 17 November 2015
energy, heat capacity, entropy and free energy are investigated. There are diverse anomalies at low
Available online 18 November 2015
temperature. In the magnetization and other thermodynamic quantities, the first-order phase transitions
Keywords: from ferromagnetic state to antiferromagnetic state and from ferromagnetic state to paramagnetic state
Heisenberg ferromagnet have been observed.
Pair approximation method
& 2015 Elsevier B.V. All rights reserved.
Phase transition

1. Introduction
Effective field theories have been discussed extensively by
many researchers to explain magnetic and thermodynamic prop-
erties obtained experimentally [1–10]. Mean field theory, being
the simplest model, corresponds to the basic cluster to be a single
spin [11]. In the model given by Oguchi [12], the cluster which is in
the interacting spin pair is dealt with. This model, called the pair
approximation method, can be limited in such a way that clusters
of the nearest-neighbor interactions can be considered. Iwashita
et al. have studied the systems with bilinear exchange interactions
and the biquadratic exchange interactions using this model [13–
17]. Phase diagram of the XXY Heisenberg ferromagnet with the
single-ion anisotropy has been investigated within the framework
of the pair approximation formulated as a variational procedure
based on the Gibbs–Bogoliubov inequality [18]. Recently much
attention has been directed to the mixed-spin systems [19–21]. In
all these theoretical works, second-nearest-neighbor exchange
interactions have not been taken into account. This method has
been extended to include both the nearest-neighbor and the sec-
ond-nearest-neighbor interactions in the Heisenberg model [22].
Moreover, some works confirm that the pair approximation
method is in good agreement with experimental results [23–25].
The negative exchange integrals can exist for some pairs of
super-exchange or super-super-exchange or indirect exchange. If
there are negative ions between positive metal ions, it may hap-
pen negative super-exchange integrals. The negative exchange has
n
Corresponding author.
E-mail address: gmert@selcuk.edu.tr (G. Mert).
been reported for Fe–Fe pairs in Sm2Fe17 and Sm2Fe17Ny which
exhibits an important difference in the critical temperature [26].
The effects of the negativity of biquadratic exchange interaction
between the nearest-neighbor pair of spins for ferromagnetic Ising
spin system on magnetization have been discussed by Iwashita
et al. [15–17]. In YMn12, antiparallel coupling must be explained by
the negative exchange integrals [27].
In this work, we will use the pair approximation method to
investigate the thermodynamic properties such as the magneti-
zation, internal energy, heat capacity, entropy and free energy of
spin-1 Heisenberg system with single-ion anisotropy on simple
cubic lattice. We suppose a negative second-nearest-neighbor
exchange interaction. The outline of this paper is as follows. In
Section 2, we present the formalism of the pair approximation
model. In Section 3, the numerical results are discussed for the
temperature dependence of magnetization, internal energy, heat
capacity, entropy and free energy. Finally, Section 4 contributes to
conclusions.
2. Model and formalism
We consider spin-1 Heisenberg ferromagnet with single-ion
anisotropy on simple cubic lattice under an external magnetic
field, which exist both nearest-neighbor and second-nearest-
neighbor interactions. We assume our Hamiltonian as follows:
H = − 2J1 ∑ Si⋅Sj − 2J2 ∑ Si⋅Si ′ − D ∑ (Siz )2 − h∑ Siz
ij ii ′ i i (1)
where the first summation runs over all nearest-neighbor pairs
and the second summation runs over all second-nearest-neighbor

http://dx.doi.org/10.1016/j.jmmm.2015.11.050
0304-8853/& 2015 Elsevier B.V. All rights reserved.
102 M. Mert et al. / Journal of Magnetism and Magnetic Materials 402 (2016) 101–104

pairs. J1 is the nearest-neighbor exchange interaction constant and have been shown both in zero external magnetic field, h/J1 ¼0, and
J2 is the second-nearest-neighbor exchange interaction constant. D in h/J1 ¼ 1. As it can be seen from this figure, at low temperatures, it
is the single-ion anisotropy parameter and h is an external mag- appears diverse anomalies and magnetization curves drop sud-
netic field applied along the z-axis. Thus, with the perspective of denly. As the absolute value of the single-ion anisotropy increases,
the pair approximation method [12], we rewrite the Hamiltonian the critical temperature decreases. When an external magnetic
(1) as field is not applied, resulting magnetization curves are shown in
Fig. 1(a). As the temperature rises, the magnetization decreases
Hp = − 2J1 Si⋅Sj − 2J2 Si⋅Si ′ − a Siz − b S zj − c Siz′
and vanishes at the critical temperature corresponding to the
− D{(Siz )2 + (S zj )2 + (Siz′)2} (2) second order phase transition. Moreover, one observes a dis-
continuities for D/J1 ¼  4 and  5 at a certain temperature. This
where
means that the first order phase transition from ferromagnetic
a = 2J1 (z1 − 1) S z + 2J2 (z2 − 1) S z + h state to antiferromagnetic state exists at kBT/J1 ¼1.6 for D/J1 ¼  4.
On the other hand, for D/J1 ¼  5, the first order phase transition
b = 2J1 (z1 − 1) Sz + h
from ferromagnetic state to antiferromagnetic state exists at kBT/
c = 2J2 (z2 − 1) Sz + h (3) J1 ¼0.65 and the second order phase transition from anti-
ferromagnetic state to paramagnetic state occurs at kBT/J1 ¼2. As
here z1 is the coordination number of the nearest-neighbor spins
we will see soon, the other thermodynamic quantities also have
and z2 is that of the second-nearest-neighbor spins. In the simple
first order phase transition at these temperatures. Similar ferro-
cubic lattice, each spin has six nearest-neighbors and 12 second-
magnetic–antiferromagnetic phase transition is found for dys-
nearest-neighbors. Sz is thermal average value of the total
prosium [28].
magnetization operator.
When an external magnetic field is applied, resulting magne-
We can get the magnetization, which is actually the statistical
tization curves are shown in Fig. 1(b). The similar anomalies have
average value of z-component of the total spin operator Sz, from
been observed at low temperatures. But, the first order phase
the definition:
transitions are not clearly. The second order phase transition
z z z − β Hp
1 Tr (Si + S j + Si ′)e temperatures from ferromagnet to paramagnet shift towards the
Sz =
3 Tre − β H p (4) high temperature region.
1
where β = (kB is Boltzmann's constant and T is the absolute
kBT 3.2. Internal energy
temperature) and Tr denotes the trace operation. Denominator in
Eq. (4) gives the partition function of the system: Internal energy of the system can be obtained from the sta-
Z = Tr (e−βHp) (5) tistical average of the Hamiltonian Hp:

We have determined temperature variations of the magneti- U = Hp (6)

zation curves by solving Eq. (4) numerically and self consistently.
Fig. 2 displays the internal energy–temperature graphic for
Thus, the other thermodynamic properties can be obtained
same parameters used in Fig. 1. In zero magnetic fields, the first
numerically.
order phase transitions appeared in Fig. 1 have been seen trivially
in this figure. For D/J1 ¼  0.1 and  1, internal energy has negative
values, while for D/J1 ¼  3,  4 and  5, it has positive values. The
3. Results and discussions
results obtained for internal energy are consistent with previous
3.1. Magnetization results given by using Green's function method [29–31].

We study the behaviors of magnetization curves for the nega- 3.3. Heat capacity
tive value of the second-nearest-neighbor interaction parameter,
J2/J1. In Fig. 1, for J2/J1 ¼  0.01, the temperature-dependences of Heat capacity is defined as the derivative of the internal energy
the magnetization curves at the various negative values of D/J1 with respect to temperature:

1.0 h/J1 = 0 1.0 h/J1 = 1

0.8 0.8 D/J1 = -0.1

-1
0.6 D/J1 = -0.1 0.6 -3
M

0.4 0.4 -4
-5
-1
0.2 -5 -3 0.2
-4

0.0 0.0

0 1 2 3 4 5 6 7 0 2 4 6 8 10 12 14
kBT/J1 kBT/J1
Fig. 1. Temperature dependence of the magnetization for the various negative values of single-ion anisotropy at J2/J1 ¼  0.01 (a) when h/J1 ¼ 0 (b) when h/J1 ¼ 1.
 M. Mert et al. / Journal of Magnetism and Magnetic Materials 402 (2016) 101–104 103

10 10

5
5
0
0 -5 -4 -3
-4 -3 -5 -1
-5
-1

U
U

-5 D/J1 = -0.1
D/J1 = -0.1 -10

-10 -15

h/J1 = 0 -20
-15 h/J1 = 1
-25
0 1 2 3 4 5 6 7 8 0 2 4 6 8 10 12 14
kBT/J1 kBT/J1
Fig. 2. Temperature dependence of the internal energy for the various negative values of single-ion anisotropy at J2/J1 ¼  0.01 (a) when h/J1 ¼0 (b) when h/J1 ¼1.

10
h/J1 = 0 8 h/J1 = 1
-4
8 -1
6
6 -5
-3 D/J1 = -0.1
C

4
4
D/J1 = -0.1
-1
-3
2 -4
2
-5

0 0
0 1 2 3 4 5 6 7 8 0 2 4 6 8 10

kBT/J1 kBT/J1
Fig. 3. Temperature dependence of the heat capacity for the various negative values of single-ion anisotropy at J2/J1 ¼  0.01 (a) when h/J1 ¼ 0 (b) when h/J1 ¼ 1.

⎛ ∂U ⎞ certain parameters, specific heat also two peaks when an external

CV = ⎜ ⎟
⎝ ∂T ⎠V (7) magnetic field is present.

In Fig. 3, we plot specific heat–temperature graphic for same 3.4. Entropy

parameters given in Fig. 1. Specific heat starts from zero. There are
discontinuities in the specific heat at temperatures corresponding Entropy can be calculated by the help of the internal energy
to the second order and first order phase transitions. Moreover, for and partition function:

4 4

3 3

D/J1 = -0.1 D/J1 = -0.1

-1 -1
2 2
S
S

-3 -3
-4 -4
-5 -5
1 1

h/J1 = 0 h/J1 = 1

0 0
0 1 2 3 4 5 6 7 8 0 2 4 6 8 10
kBT/J1 kBT/J1
Fig. 4. Temperature dependence of the entropy for the various negative values of single-ion anisotropy at J2/J1 ¼  0.01 (a) when h/J1 ¼0 (b) when h/J1 ¼ 1.
104 M. Mert et al. / Journal of Magnetism and Magnetic Materials 402 (2016) 101–104

0
h/J1 = 0 h/J1 = 1
0
-5
-5 -5
-5 -4
-10 -4
-10 -3
-3
-1 -15
F

F
-15

D/J1 = -0.1 -20 -1

-20
D/J1 = -0.1
-25 -25

-30 -30
0 1 2 3 4 5 6 7 8 0 2 4 6 8 10

kBT/J1 kBT/J1
Fig. 5. Temperature dependence of the free energy for the various negative values of single-ion anisotropy at J2/J1 ¼  0.01 (a) when h/J1 ¼ 0 (b) when h/J1 ¼1.

S = kB ln Z + kBβ U (8) antiferromagnetic state and from ferromagnetic state to para-

magnetic state. Moreover, the other thermodynamic properties
In Fig. 4, we plot the entropy–temperature graphic for same such as internal energy, specific heat, entropy and free energy also
parameters given in Fig. 1. The entropy has zero value at zero
have both first order and second order phase transitions.
temperature. As the temperature increases, entropy increases until
a constant value. There are discontinuities at the first order phase
transition temperatures. When an external magnetic field is ap-
plied, the entropy curves at the critical temperatures are blunted. References

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