Applied Mathematical Modelling 30 (2006) 545553

www.elsevier.com/locate/apm

Numerical stochastic model for the magnetic relaxation time

of the ne particle system with dipolar interactions
Mihaela Osaci *, Manuela Panoiu, Teodor Heput, Ionel Muscalagiu
Technical University of Timisoara, Hunedoara Engineering Faculty, 5 Revolutiei Street, Hunedoara 331128, Romania
Received 1 September 2003; received in revised form 1 October 2005; accepted 1 November 2005
Available online 27 December 2005

Abstract
This paper presents the results obtained by numerical simulations, the magnetic relaxation time simulation for a ne
particle system with dipolar magnetic interaction. We used a 3D simulation model for ne magnetic particles with spherical
shape and lognormal distribution for their diameters. Starting from DormannBessaisFiorani model, the 3D model we
used is more realistic if we consider that the particles are randomly arranged into a preset volume, following a Gaussian
distribution generated with the BoxMueller transformation.
Concerning the dependency of the average relaxation time on temperature and on the dispersion of the particle diameters logarithm, the analysis is achieved for three cases: without interaction, weak dipolar magnetic interaction, and strong
dipolar magnetic interaction between particles. We found that the average relaxation time for the ne particle system
decreases by temperatures increasing and the average relaxation time grows by the growth of the dispersion of the random
ln d variable.
 2005 Elsevier Inc. All rights reserved.
PACS: 72.15.Lh; 75.50.Tt; 78.20.Bh
Keywords: Numerical simulation; Relaxation time; Relaxation process; Fine particles; Dipolar interaction

1. The 3D model for numerical simulation of magnetic relaxation time for a ne particle system with dipolar
interaction
In the case of a ne particle assembly, when analyzing magnetization and demagnetization, it is very important to consider the dipolar magnetic interaction between particles. When this interaction is included, the
problem becomes very complex and, until now, there is no analytic solution exactly known [1].
We considered a 3D model for ne magnetic particles with single-axis anisotropy, spherical shape and randomly distributed in a given volume. It is considered that the particle system is placed in an external magnetic

Corresponding author. Tel.: +40 254 207533; fax: +40 254 207501.
E-mail address: m.osaci@h.utt.ro (M. Osaci).

0307-904X/$ - see front matter  2005 Elsevier Inc. All rights reserved.
doi:10.1016/j.apm.2005.11.013

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M. Osaci et al. / Applied Mathematical Modelling 30 (2006) 545553

~i and m
~j
eld. Initially, all magnetic moments are assumed parallel with their anisotropy axis. Let us consider m
be the magnetic moments of the particles i and j, respectively.
The study of the particle systems behavior begins at the moment when the external magnetic eld is turned
o (t = 0). In these conditions, the total energy of the system is equal to the sum of the total anisotropy energy
and the dipolar magnetic interaction energy.
In order to follow the general approach presented in [4], which starts from the dipolar magnetic interaction
energy between two particles i and j in spherical coordinates (see Fig. 1) and use of an average over the azimuthal
angles ui and uj, results in the introduction of the magnetic dipolar contribution to the i particles energy:
X mj
l
Eid  0 mi cos hi
3z2ij  1 cos hj ;
1
3
4p
r
ij
j6i
where rij is the magnitude of the vector that connects the center of the particles i and j, and zij is the component
_
~
r
along the z-axis of the unit vector r ij rijij .
Assuming that the particle system has single-axis anisotropy, the following relation gives the total energy of
the ith particle:
X mj
l
Ei Eid Ea  0 mi cos hi
3z2ij  1 cos hj  Kv cos2 hi ;
2
3
4p
r
ij
j6i
where Eid is the dipolar contribution from the i particles energy, Ea is the anisotropy energy, K is the singleaxis anisotropy constant for the particles and v is the particles volume.
2. The spherical particle system with lognormal distribution of diameter
In the case of spherical particles with lognormal distribution of their diameters, the magnetic moments for i
and j particles are:
m i vi M s

and

mj vj M s ;

where Ms is the spontaneous magnetization for a particle and vi and vj are the volumes of i and j particles,
respectively.
Based on Eqs. (2) and (3), the dipolar contribution from the i particles energy can be written as
Eid 

n
X
vj 3z2ij  1
l0
vi M 2s cos hi
cos hj .
4p
r3ij
j1

j6i

We introduce the following notation:

H Li cd 3i

n
X
d 3j 3z2ij  1
cos hj ;
r3ij
j1

j6i

where
c

l0 pM 2s
144

z
i

anisotropy axis
j

mi

ij

i
i

x
Fig. 1. Model for two particles.

mj

M. Osaci et al. / Applied Mathematical Modelling 30 (2006) 545553

547

is a constant. Here n is the number of particles in the system, di and dj are the diameters of i and j particles,
respectively.
For a system made of interacting nano-particles of the same material, during the ip of the moment of one
of the particles the system is not in thermal equilibrium. It is not simple to describe the non-equilibrium properties of the interacting system during this ip process and, therefore, in the rst approximation we consider
that the orientation of the magnetic moment of the j particle does not change. Then, in Eq. (5), cos hj is a
parameter. Using (5), the dipolar component of the energy of the i particle becomes:
Eid H Li cos hi

and the total energy of the i particle is

Ei H Li cos hi 

Kp 3
d cos2 hi .
6 i

Eq. (8) shows that the energy Ei can have, if qi 3H Li =Kpd 3i < 1, one or two minima and, in the latter
case, there is a maximum between them at hi arccos3H Li =Kpd 3i . Furthermore, because:
Emax

3H 2Li
;
2Kpd 3i

Emin 1 H Li 

Kpd 3i
;
6

Emin 2 H Li 

Kpd 3i
6

the energy barriers [1] become:

DEb1i Emax  Emin 1

3H 2Li
Kpd 3i
;

H

Li
6
2Kpd 3i

10

DEb2i Emax  Emin 2

3H 2Li
Kpd 3i
.

Li
6
2Kpd 3i

11

For qi P 1 there is present only one minimum and one maximum, and the energy barrier is
DEbi 2H Li .

12

Each particle system has two stable orientations, separated by energy barriers given by the relations (10) or
(11) for qi < 1 and (12) for qi P 1.
The probability per time unit that a particle jumps from one stable state to another is given by:


DEbi
P Ebi f0 exp 
13
if qi > 1;
kBT




DEb1i
DEb2i
P Ebi f0 exp 
14
f0 exp 
if qi < 1;
kBT
kBT
where f0 is a constant which we assume to be f0 109 s1.
The relaxation time for the particle system i is
si

1
.
P Ebi

15

3. HLi size computing

We will give a numerical method of simulation of the HLi size in relation (5). In this case, we suppose that
the particles are randomly distributed in the considered volume. We also assume that the z-components of the
unit vectors along the direction between the particle i and another particle j, zij, have a Gaussian distribution
in (0, 1) domain with zmed = 0.5. We generate this distribution with the BoxMueller transformation [2]:
p
16
zij zmed rzz  lnrand1  cos2p  rand2 sin2p  rand2;
where rand1 and rand2 are two random numbers with uniform distribution in (0, 1) domain and rzz is the variance of the zij variable.

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M. Osaci et al. / Applied Mathematical Modelling 30 (2006) 545553

We assume that (rxij, ryij, rzij) are the components of the~

rij vectors that connect the center of i and j particles.
r2ij r2xij r2yij r2zij .

17

The rxij, ryij, rzij components are generated by means of the BoxMueller transformation:
p
rxij rxmed rx  lnrand1  cos2p  rand2 sin2p  rand2;
p
ryij rymed ry  lnrand1  cos2p  rand2 sin2p  rand2;
p
rzij rzmed rz  lnrand1  cos2p  rand2 sin2p  rand2;

18
19
20

rx, ry and rz are the variances of the rxij, ryij and rzij, respectively, by the average values rxmed, rymed, rz med.
We also assume that uj variables, uj = cos h,j which represent the cosines of the angle between the magnetic
moment of the particle j, and its anisotropy axis has a Gaussian distribution with variance ru generated by
means of the BoxMueller transformation:
p
21
uj ru  lnrand1  cos2p  rand2 sin2p  rand2.
After the generation of these variables, the HLi size for the i particle can be computed by using the following
relation:
n1
X
d 3j 3z2ij  1
22
H Li cd 3i
q3  uj .
j1
r2xij r2yij r2zij
4. Numerical simulation method, results and models optimization
The simulations were performed on a system with n = 270 spherical magnetite ne particles with anisotropy
constant K = 19,000 J/m3, spontaneous magnetization Ms = 4.7 105 A/m, and with most probable value of
the particle diameter dm = 9.848 nm.
The particles rst-order neighbors for i particle, for a very high density system, are the neighbors that are
placed at one diameter distance from the central point of the i particle (Fig. 2).
Using [3], if we note with
V powder
f
23
V test
the volume fraction of particles, for a high density system we can write
24

f 0:32  f0 ;
with
f0

8Kp
.
l0 M 2s

25

I ord.
II ord.
III ord.

Fig. 2. Orders of the nearest neighbors for a very high density system.

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549

Using (23)(25), we generally obtain the number of k order neighbors by using the following relation:
3

nk 0:322k 1 f0 .

26

For the diluted systems, we keep the number of neighbors of I, II and III order and we use a parameter
D distance between two particles one next to each other (not between their central points), which is bigger
as the system is more diluted (see Fig. 3).
In the rst approximation, we considered that the particles are of the same diameter.
We note rx,k = vr rxmed,k, ry,k = vr rymed,k, rz,k = vr rzmed,k the variance of the components rxij, ryij, rzij, k
being the order of the nearest neighbors for a given particle i.
These calculations are performed under the hypothesis of weak or strong dipolar interaction. In the weak
interaction case, which corresponds to a concentration of the particles of 2.24 1023 part/m3, the distance
between the i particle and the nearest neighbors is 2dm, 4dm to the next nearest neighbors, and 6dm to the
third-order particles. For a strong interaction, which corresponds to a concentration of the particles of
1.16 1024 part/m3 the distance between the i particle and the nearest neighbors is dm, 2dm, and 3dm, respectively.
If we follow the dependency of the average relaxation time according to the number of the particles in the
system at 300 K for variance of the distribution of the variable uj = coshj, ru = 0.4 and dierent values of the
variance rx,k, ry,k, rz,k, dierent values of the parameter vr Figs. 4 and 5, we can observe that the average
relaxation time depends on the vr parameter of the distributions variations of the distances between the given
particle i and the other particles of the system and presents uctuations with the number of particles from
vr = 0.4 for the system of strong interactions. These observations determine the choice of the vr parameter
of the distributions variations of the distances between the given particle i and the other particles of the system towards the 0.3 value, if the system of strong interactions is also studied. For the simulations we are going
to perform, we chose vr = 0.05.

D
2d+D
Fig. 3. The rst order of the nearest neighbors for a diluted system.

Fig. 4. The dependency of the average relaxation time on the number of neighbor particles taken into calculation in the system at 300 K:
(1) without interaction, (2) weak interaction and (3) strong interaction.

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M. Osaci et al. / Applied Mathematical Modelling 30 (2006) 545553

Fig. 6 presents the dependency of the average relaxation time on the number of particles taken into account
and to the variance of the distribution of the variable uj = cos hj at the temperature of 300 K for the system of
strong interaction. The distribution parameter of the distances between the particle i and the other particles in
the system is xed to vr = 0.05.
It can be seen in Fig. 6 that the variation of the distribution for the random variable uj = cos hj inuences in
a slight manner the average relaxation time. Taking into account this estimated study, the simulations that
follow will be done for the parameter vr = 0.05 of the distribution variances of the distances between the given
particle i and the other particles of the system and the distribution variance of the angles ru = 0.4.
Now, we consider that particle dimensions have a lognormal distribution. For the generation of random
values of particle diameters, we used the algorithm presented in [46]. The method of generating a lognormal
distribution is based on the relation
d i erln d ui ln d 0 ;

27

Fig. 5. The dependency of the average relaxation time on the number of neighbor particles taken into calculation in the system at 300 K:
(1) without interaction, (2) weak interaction and (3) strong interaction.

Fig. 6. The dependency of the average relaxation time on the number of particles taken into account and on the variance of the
distribution of the variable uj = cos hj for the system of strong interaction at the temperature of 300 K and vr = 0.05.

M. Osaci et al. / Applied Mathematical Modelling 30 (2006) 545553

551

where ui are the values of a normal distribution on (0, 1), with the mean equal to ln d0 and the variance equal to
r2ln d .
In Eq. (27), we have considered that the mean of the distribution is ln d0 = 18.4409 and the variance is
r2ln d 0:01 rln d 0:1. The most probable value of the particle diameter dm = 9.848 nm corresponds to a
volume of 5 1025 m3.
In the simulation algorithm, we rst generate the random variables, which are used in the model, and then
we computed the HLi size on the particles by using Eq. (22) and the energy barriers of each particle by using
Eqs. (10)(12). Finally, from Eq. (10), the time relaxations and the average time relaxation.
5. The average time relaxation analysis
Fig. 7 shows the dependency of the average relaxation time on temperature.

Fig. 7. The dependency of the average relaxation time on temperature for the two kinds of interactions: (1) without dipolar interaction, (2)
with weak dipolar interaction and (3) with strong dipolar interaction.

Fig. 8. The dependency of the average relaxation time on the variance of the logarithm for the particle diameters for 100 neighbor particles
at 300 K: (1) without interaction, (2) weak interaction and (3) strong interaction.

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M. Osaci et al. / Applied Mathematical Modelling 30 (2006) 545553

It is shown in Fig. 7 that the average relaxation time for the ne particle system decreases when the temperature increases.
Figs. 810 show the dependency of the average relaxation time on the logarithm of the variance of the particle diameters for 100, 150 and 200 neighbor particles at 300 K. In these gures vr = 0.05 and ru = 0.4.
From Figs. 8 to 10, it may be seen that the average relaxation time increases with the growth of the dispersion of the random variable.
Finally we compared the simulated results to the model presented in this paper and also to the models from
the literature: NeelBrown, DormannBessaisFiorani and MorupTronc [1,7] Fig. 11 for ne magnetite
particles at 300 K with rln d = 0,1.
In Fig. 11, it can seen that below r = Kv/kBT = 2.65 the resulted values obtained by using the model presented in this paper are situated between the resulted values obtained by DormannBessaisFiorani and
MorupTronc models.

Fig. 9. The dependency of the average relaxation time on the variance of the logarithm for the particle diameters for 150 neighbor particles
at 300 K: (1) without interaction, (2) weak interaction and (3) strong interaction.

Fig. 10. The dependency of the average relaxation time on the variance of the logarithm for the particle diameters for 200 neighbor
particles at 300 K: (1) without interaction, (2) weak interaction and (3) strong interaction.

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Fig. 11. The dependency between s/s0 and Kv/kBT with present model (2), with MorupTronc model (3), with DormannBessaisFiorani
model (1) and with NeelBrown model (4).

6. Conclusions
In this paper a simulation has been carried out to determine the dependency of the average relaxation time
for a ne particle system on the temperature, on the natural logarithm variance of diameters and on the particle volume. Based on DormanBessaisFiorani model [1], there has been proposed a 3D model, similar to a
real situation. In this model it has been considered that the particles are randomly arranged in a volume, with
a Gaussian distribution generated by means of the BoxMueller relation. It has been also considered that hj
angles are random Gaussian variables.
Considering the dipolar magnetic interaction between particles, there can be observed an inuence for the
dependency between average relaxation time and the temperature. It results in an increase of the average relaxation time by temperatures decreasing. The increase is less signicant when the dipolar magnetic interaction is
strong.
It is observed in Figs. 68 that the average relaxation time is inuenced by the dipolar interaction strength
and also by the natural logarithm variance of particle diameter.
References
[1]
[2]
[3]
[4]
[5]

M.F. Hansen, S. Morup, Journal of Magnetism and Magnetic Materials 184 (1998) 262274.
H.M. Petersen, R.G. Koch, P.H. Swart, R. van Heereden, IEEE Transactions on Power Delivery (1995) 17331740.
J. Garcia-Otero, M. Porto, J. Rivas, A. Bunde, Physical Review Letters 84 (1) (2000) 167170.
S.M. Ermakov, Monte Carlo Method and Connected Problems, Technique Publishing, Bucharest, 1976, pp. 3657.
I. Sacuiu, D. Zorilescu, The Random Numbers, Applications in Economy, Industry and in the Study of Natural Phenomenon,
Academy Publishing, Bucharest, 1978, pp. 4347.
[6] I. Mihoc, Calculus of Probability and Mathematical Statistics, Babes-Bolyai University Publishing, Cluj-Napoca, 1994, pp. 3657.
[7] L. Neel, Annales de Geophysique 5 (2) (1949) 99136.