Physica B 532 (2018) 144–148

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Physica B
journal homepage: www.elsevier.com/locate/physb

Factors on the magnetic properties of the iron nanoparticles by classical MARK

Heisenberg model
⁎
Trong Dung Nguyena, , Chinh Cuong Nguyena, The Toan Nguyenb, Khac Hung Phamc
a
Faculty of Physics, Hanoi National University of Education, 136 Xuan thuy, Cau giay, Ha Noi, Vietnam
b
Faculty of Physics, VNU University of Science, Ha Noi, Vietnam
c
School of Engineering Physics, Hanoi University of Science and Technology, Dai Co Viet, Ha Noi, Vietnam

A R T I C L E I N F O A BS T RAC T

Keywords: In this paper, we used the Monte-Carlo simulation technique to investigate the magnetic properties of the
Particle size effects samples of amorphous iron material which could be described as a spin Heisenberg system. The exchange
Core/shell model interaction is taken into account as a function of the distance between the two spins. The results showed the
Transition temperature existence of the magnetic phase transition behavior of the nanoparticles. The phase transition temperature
Iron nanoparticles
obtained by our simulations and the semi-empirical calculations are well matched. The magnetization of the
Magnetism
core/shell system strongly depends on the shell thickness when the spins on the interface of the core and the
Classical Heisenberg model
shell layer are frustrated. The transition temperature seems to be independent on the structure of the shell.

1. Introduction covered by a non-magnetic layer such as gold, silver or polymer, etc.

Theoretically, the material could be described by a core/shell model.
Iron is a ferromagnetic material with very high magnetic moment So, one could evaluate the magnetization of the core and the shell
(around 220 emu/g). It is well known that the crystal structure of the layers individually [31,32]. A simple model was introduced to calculate
bulk iron is body-centered cubic (BCC) with critical temperature from the magnetization of the core and the shell of nanoparticles [33], in
1043 to 1881 K (corresponding to the structural shifts from α (1185 K) which, the magnetic core consists of the Ising spins. The simulation
→γ (1667 K) →δ (1811 K) isomorph) [1]. Iron and its alloys are widely results are in good agreement with the results from semi-empirical
involved in many fields of science and technology [2]. In particular, calculations [34,35].
nanoscale ferromagnetic iron materials are used in many spintronic For the bulk Fe with BCC structure, it has Curie phase transition
devices including large-capacity memory [3], magnetic resonance temperature Tc = 1043 K [30,36,37], that is lower in the case of thin
imaging [4], nonlinear optics [5], sensors [6], catalysts [7], biomedical films and strongly depends on the film thickness [38,39]. Especially, for
tools such as separation of biomolecules, drug carriers, cell sensing etc. the amorphous iron material, the transition temperature is still lower
[8,9] and other pharmaceutical applications [10]. Therefore, these than the one of the bulk even though it is put in an external magnetic
materials attract a great attention of researchers in both theoretical and field [40]. We have recently studied the dynamical properties of the
experimental studies [11]. magnetic nanoparticles as: Fe, FeB and Ni [41–43]. The simulation
The ferromagnetic materials have been theoretically studied by results were verified by the experimental data for iron material [44].
various methods such as: the mean-field theory [12], the effective-field Although the dynamical and structural properties of these amor-
theory [13], the effective mean-field theory, the Green-function method phous nanoparticles have been studied by the molecular dynamics
[14,15], the Monte Carlo (MC) simulations [15,16], the contingent simulations in the previous work [41,43,45,46], its magnetic properties
valuation method (CVM) [17] and the Bethe model [18]. During recent have not been investigated yet. Therefore, it is necessary to use Monte
years, the studies of influence of nanoparticle size on Curie tempera- Carlo simulation and the classical Heisenberg model to study the effect
ture are only based on the semi-empirical models [19]. The results have of system size and the competitive interaction between the spins on the
shown that the Curie temperature decreases with decreasing the behavior of magnetic phase transition. The influences of the shell
nanoparticle size [19–26]. The semi-empirical expressions have been structure on the phase transition behavior were investigated by varying
modified for some applications in the different models [27–30]. the shell thickness and the exchange interaction of the spins in the shell
In the biomedical applications, the ferromagnetic nanoparticles are layer.

⁎
Corresponding author.
E-mail address: [email protected] (T.D. Nguyen).

http://dx.doi.org/10.1016/j.physb.2017.08.083
Received 27 March 2017; Received in revised form 31 July 2017; Accepted 30 August 2017
Available online 01 September 2017
0921-4526/ © 2017 Elsevier B.V. All rights reserved.
T.D. Nguyen et al. Physica B 532 (2018) 144–148

Fig. 1. The average energy (a), normalized magnetization (b), specific heat (c) and magnetic susceptibility (d) as a function of temperature for several values of system sizes
(500, 1000, …, 20000) .

2. Calculation method In this work, we use the standard Monte-Carlo simulation method
to calculate the physical quantities as functions of temperature T. These
We consider a model of spherical core/shell nanoparticle is con- quantities that are defined below:
structed of the amorphous ferromagnetic materials with a fixed bulk
density. Let D denote the diameter of the particle which can be 1 1
〈E 〉 = 〈 〉; 〈m〉 = ∑ Si
evaluated by N N i (4)
⎛ 3N ⎞1/3 are the internal energy and normalized magnetization per spin. From
D = 2⎜ ⎟ ,
⎝ 4πρ ⎠ (1) the expression above, one can evaluate the specific heat and magnetic
susceptibility by
with ρ = (N / V ) = 7.0 g/cm3 is the density. N and V are the total number
of atoms and the volume of the particle. These samples were generated 〈E2〉 − 〈E 〉2 〈m2〉 − 〈m〉2
Cv = N ; χ=N .
by MD simulations with the Pak-Doyama pair interaction potential and (kB T )2 kB T (5)
a free boundary condition [41]. For the magnetic material, with increasing the temperature, the
In order to study the magnetic property of this system, we assume system undergoes from ordered to dis-ordered phases. The phase
that each atom has only one spin vector Si of unit modulus |Si | = 1. transition temperature Tc is approximately estimated at the maximum
Therefore, the system is equivalent to a classical Heisenberg spin model of specific heat Cv. On the other hand, the critical temperature of the
and its Hamiltonian can be written as [40,47,48]: spherical nanoparticles can be evaluated by the semi-empirical expres-
sion [29,30,49–51]:
 =− ∑ Jij (rij )(Si ·Sj ),
rij ∈ R (i ) (2) ⎛ 1 ⎞ ⎛ 2SB 1 ⎞
Tc (D ) = T0 ⎜1 − ⎟ exp ⎜ − ⎟.
in which, rij = |ri − rj | is the distance between the spins and the sum ⎝ (2D / ch ) − 1 ⎠ ⎝ 3NA (2D / ch ) − 1 ⎠ (6)
takes over all the spins inside a sphere of radius R(i) centered on Si . In which, D is the diameter of the particle. T0 and SB is the critical
Note that, the amorphous materials are not “fully” crystalline such as temperature and evaporation entropy of the bulk material (D → ∞)
crystal lattices (sc, fcc, bcc, etc). So, we have to define the exchange respectively. c and h are the constants of the material.
interaction Jij (rij ) as a function of the distance between the spins NA = 8.314 J/mol·K is the Avogadro constant.
[47,49] All simulations are performed for the sufficient run times in order
⎛ rij ⎞3 to reduce the statistical errors. The equilibrating time is about 106 MC
Jij (rij ) = J0 ⎜1 − ⎟ Θ (rc − |rij |), steps/spin and the averaging time is 2 × 10 6 MC steps/spin.
⎝ rc ⎠ (3)

where rc is the cut-off radius which is determined up to the third 3. Results and discussions
nearest-neighbor distance. Θ (rc − |rij |) is the Heaviside step function. J0
is a constant in unit of energy depending on the pair of spins (Si , Sj ), In this section, we present the simulation results that were
i.e., J0 ≡ Jc / s if both spins are in the core/shell layers; J0 ≡ Jcs if one is in performed on the model of the ferromagnetic nanoparticles generated
the core and other one is in the shell. by the iron atoms. Some theoretical and experimental parameters have

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T.D. Nguyen et al. Physica B 532 (2018) 144–148

been used such as: the coupling energy Jc = 0.9049 eV , the cut-off
radius for the exchange interaction distance rc = 0.375 nm [49]. For the
Eq. (6), we used the parameters: T0 = 1043 K , SB = 111.52 J/mol·K , c =
0.5 and h = 0.2483 nm [51].

3.1. Core-only nanoparticles

We investigate the size dependence of the phase transition tem-

perature of the nanoparticles without the shell layer. We consider the
system sizes N = 300, 500, 700, 1000, 2000, …, 20000 atoms which
correspond to the diameter of the particles
D = 2.12, 2.49, 2.88, 3.25, 4.07, …, 8.39 nm , respectively.
In Fig. 1, the thermodynamic quantities are presented as a function
of temperature for the different values of N. Note that, the error bars
were not included into the figures because the errors are smaller than Fig. 2. The transition temperature versus the diameter of nanoparticles. The circles
the symbol sizes. In the ordered phase T < Tc , the normalized magne- (with error bars) are the simulation data in Table 1 and the solid line is plotted using the
tization increases with increasing the system sizes (Fig. 1b). Whereas, it expression (6).
decreases with increasing N for T > Tc . This observation is one of the
conditions to suggest the existence of a phase transition in the +1.0Jc to −1.0Jc are shown in Fig. 4. The increase in Js of the shell layer
magnetic system. In addition, Figs. 1c and 1d clearly show that the is equivalent to the increase in size of the core. Hence, the total
maximum value of both Cv and χ that increase with increasing the magnetization is also larger. It is an interesting observation that the
particle size. So, we can conclude that our samples of magnetic transition temperature seems to be unchanged for all the considered
nanoparticles exhibit a single phase transition. cases and all the peaks of specific heat locate at the same positions
Next, we estimate the phase transition temperature Tc for each (Figs. 3b and 4b). For instance, Fig. 4b, whose behavior is also
particle size by interpolating the maximum of the specific heat. These observed in the plots of magnetic susceptibility.
results are listed in Table 1 including the transition temperature Tse Similarly, we consider the case Jcs = −1.0Jc . The effects of the shell
evaluated by the expression (6) for the comparison. thickness and the exchange interaction of the spins in the shell layer on
Fig. 2 clearly shows an excellent agreement between the simulation the phase transition are shown in Figs. 5 and 6. The magnetization
data and that of the semi-empirical calculations in acceptable error strongly depends on d (Fig. 5a). Because the competitive interaction
limits. between the spins on the interface of the core and the shell layers, the
The simulation results not only fit to the data of the semi-empirical spins arrange in the opposite directions. Therefore, the magnetic
calculations, but they are also consistent with the simulation for the moment of the shell reduces the total magnetization of the system.
bulk and thin films [30,37–39]. Fig. 6a shows that the magnetization does not depend on Js > 0 and the
same also for a case Jcs =+ 1.0Jc . Moreover, the independence of the
transition temperature on the shell thickness and the exchange
3.2. Core/shell nanoparticles
interaction Js (see in Figs. 5b and 6b) was again observed.
Next, we investigate the effects of the shell thickness (denoted by d)
on the magnetization and the transition temperature of the magnetic 4. Conclusions
nanoparticles. The particle has a core with a fixed size of diameter of
2.8 nm. The thickness of the shell layer is 0.1, 0.2, 0.3 and 0.4 nm. The In this paper, we directly used the sample structures of iron
exchange interaction between the spins of the core is still unchanged material that are generated by MD simulations instead of the common
Jc = 0.9049 eV while the other interactions are varied (in unit of Jc) for lattice models. The magnetic properties of the nanoparticles were
all simulations. investigated by applying the core/shell model with the Heisenberg
We consider the case of Jcs =+ 1.0Jc (ferromagnetic interaction spins. The physical quantities ware obtained by the Monte-Carlo
between the spins of the core and the shell). For Js = −0.6Jc , the simulations.
normalized magnetization and specific heat reduce with increasing the For the case of core-only nanoparticles, the system has a single
shell thickness due to the competition between ferromagnetic and phase transition. The transition temperature is estimated as a function
antiferromagnetic interactions of the spins in the core and shell layers of the diameter of spherical magnetic particle. The simulation result is
(see in Fig. 3). the best fit to the semi-empirical expression [29,30,50,51]. It is
For a fixed shell thickness d = 0.2 nm , the results obtained by confirmed that the Eq. (6) is not only applicable to the lattice materials,
varying the exchange interaction of the spins in the shell layer from but also to the amorphous nanoparticles.
We have investigated the influences of the shell thickness and the
Table 1
exchange interaction on the phase transition. We find that the kind of
The transition temperature obtained by the simulations Tc and the semi-empirical
calculations Tse for several values of N.
interaction of the spins on the interface between the core and the shell
layers plays an important role in controlling the total magnetization of
System size N 300 500 700 1000 2000 3000 nanoparticles. An interesting observation is that the transition tem-
perature does not depend on the shell configurations. The results are
Diameter D (nm) 2.12 2.49 2.88 3.25 4.07 4.68
Tc (K) 767 ± 6 808 ± 6 832 ± 8 855 ± 7 895 ± 6 914 ± 5
not only in good agreement with those obtained in the bulk and thin
Tse (K) 773 809 838 859 894 912 films [30,40,39,52] but also are the samples of the design and
[29,30,50,51] biomedical applications of magnetic nanoparticles.
System size N 4000 5000 10000 15000 20000
Diameter D (nm) 4.98 5.30 6.60 7.77 8.39
Tc (K) 919 ± 4 930 ± 6 950 ± 6 959 ± 5 965 ± 5
Acknowledgement
Tse (K) 920 927 949 968 968
[29,30,50,51]
We thank V. Thanh Ngo for helpful comments and suggestions.

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Fig. 3. The magnetization (a) and specific heat (b) vs temperature for several values of the shell thickness with Jcs =+ 1.0Jc and Js = −0.6Jc .

Fig. 4. The magnetization (a) and specific heat (b) versus temperature for several Js with Jcs =+ 1.0Jc and d = 0.2 nm.

Fig. 5. The magnetization (a) and specific heat (b) vs temperature for several values of the shell thickness with Jcs = −1.0Jc and Js =+ 0.6Jc .

Fig. 6. The magnetization (a) and specific heat (b) versus temperature for several Js with Jcs = −1.0Jc and d=0.2 nm.

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