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www.elsevier.com/locate/apm

**Numerical stochastic model for the magnetic relaxation time
**

of the ﬁne particle system with dipolar interactions

Mihaela Osaci *, Manuela Pa˘noiu, Teodor Heputß, Ionel Muscalagiu

Technical University of Timisßoara, 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 ﬁne

particle system with dipolar magnetic interaction. We used a 3D simulation model for ﬁne magnetic particles with spherical

shape and lognormal distribution for their diameters. Starting from Dormann–Bessais–Fiorani 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 Box–Mueller transformation.

Concerning the dependency of the average relaxation time on temperature and on the dispersion of the particle diameter’s 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 ﬁne particle system

decreases by temperature’s 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 ﬁne particle system with dipolar

interaction

In the case of a ﬁne 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 ﬁne 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@ﬁh.utt.ro (M. Osaci).

**0307-904X/$ - see front matter 2005 Elsevier Inc. All rights reserved.
**

doi:10.1016/j.apm.2005.11.013

(2) and (3). Model for two particles. the total energy of the system is equal to the sum of the total anisotropy energy and the dipolar magnetic interaction energy. results in the introduction of the magnetic dipolar contribution to the i particle’s energy: X mj l Eid ¼ 0 mi cos hi ð3z2ij 1Þ cos hj . 1) and use of an average over the azimuthal angles ui and uj. The spherical particle system with lognormal distribution of diameter In the case of spherical particles with lognormal distribution of their diameters. ð2Þ 3 4p r ij j6¼i where Eid is the dipolar contribution from the i particle’s energy. ð3Þ where Ms is the spontaneous magnetization for a particle and vi and vj are the volumes of i and j particles. Osaci et al. the dipolar contribution from the i particle’s energy can be written as Eid ¼ n X vj ð3z2ij 1Þ l0 vi M 2s cos hi cos hj . / Applied Mathematical Modelling 30 (2006) 545–553 ~i and m ~j ﬁeld. K is the singleaxis anisotropy constant for the particles and v is the particle’s volume. respectively. respectively. Initially. 4p r3ij j¼1 ð4Þ j6¼i We introduce the following notation: H Li ¼ cd 3i n X d 3j ð3z2ij 1Þ cos hj . ð1Þ 3 4p r ij j6¼i where rij is the magnitude of the vector that connects the center of the particles i and j. the magnetic moments for i and j particles are: m i ¼ vi M s and mj ¼ vj M s . In order to follow the general approach presented in [4]. Assuming that the particle system has single-axis anisotropy. the following relation gives the total energy of the ith particle: X mj l Ei ¼ Eid þ Ea ¼ 0 mi cos hi ð3z2ij 1Þ cos hj Kv cos2 hi . all magnetic moments are assumed parallel with their anisotropy axis. ϕj → mj . The study of the particle system’s behavior begins at the moment when the external magnetic ﬁeld is turned oﬀ (t = 0). 2. r3ij j¼1 ð5Þ j6¼i where c¼ l0 pM 2s 144 ð6Þ z θi anisotropy axis θj → mi → ij r i ϕi j y x Fig.546 M. 1. Based on Eqs. and zij is the component _ ~ r along the z-axis of the unit vector r ij ¼ rijij . In these conditions. which starts from the dipolar magnetic interaction energy between two particles i and j in spherical coordinates (see Fig. Let us consider m be the magnetic moments of the particles i and j. Ea is the anisotropy energy.

M. because: Emax ¼ 3H 2Li . where rand1 and rand2 are two random numbers with uniform distribution in (0. in the latter case. þ H þ Li 6 2Kpd 3i ð11Þ For qi P 1 there is present only one minimum and one maximum. It is not simple to describe the non-equilibrium properties of the interacting system during this ﬂip process and. zij. Then. separated by energy barriers given by the relations (10) or (11) for qi < 1 and (12) for qi P 1. We generate this distribution with the Box–Mueller transformation [2]: pﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃ ð16Þ zij ¼ zmed þ rzz lnðrand1Þ ½cosð2p rand2Þ þ sinð2p rand2Þ. P ðEbi Þ ð15Þ 3. kBT kBT where f0 is a constant which we assume to be f0 ﬃ 109 s1. 6 Emin 2 ¼ H Li Kpd 3i 6 ð9Þ the energy barriers [1] become: DEb1i ¼ Emax Emin 1 ¼ 3H 2Li Kpd 3i . we suppose that the particles are randomly distributed in the considered volume. di and dj are the diameters of i and j particles. have a Gaussian distribution in (0. respectively. therefore. H þ Li 6 2Kpd 3i ð10Þ DEb2i ¼ Emax Emin 2 ¼ 3H 2Li Kpd 3i . the dipolar component of the energy of the i particle becomes: Eid ¼ H Li cos hi ð7Þ and the total energy of the i particle is Ei ¼ H Li cos hi Kp 3 d cos2 hi . and the energy barrier is DEbi ¼ 2H Li . (5). there is a maximum between them at hi ¼ arccosð3H Li =Kpd 3i Þ. 1) domain and rzz is the variance of the zij variable. The relaxation time for the particle system i is si ¼ 1 . kBT DEb1i DEb2i P ðEbi Þ ¼ f0 exp ð14Þ þ f0 exp if qi < 1. In this case. 6 i ð8Þ Eq. ð12Þ Each particle system has two stable orientations. (8) shows that the energy Ei can have. HLi size computing We will give a numerical method of simulation of the HLi size in relation (5). Using (5). in Eq. Here n is the number of particles in the system. if qi ¼ ð3H Li =Kpd 3i Þ < 1. 2Kpd 3i Emin 1 ¼ H Li Kpd 3i . during the ﬂip of the moment of one of the particles the system is not in thermal equilibrium. / Applied Mathematical Modelling 30 (2006) 545–553 547 is a constant.5. For a system made of interacting nano-particles of the same material. 1) domain with zmed = 0. The probability per time unit that a particle jumps from one stable state to another is given by: DEbi P ðEbi Þ ¼ f0 exp ð13Þ if qi > 1. . in the ﬁrst approximation we consider that the orientation of the magnetic moment of the j particle does not change. We also assume that the z-components of the unit vectors along the direction between the particle i and another particle j. cos hj is a parameter. one or two minima and. Furthermore. Osaci et al.

rzij components are generated by means of the Box–Mueller transformation: pﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃ rxij ¼ rxmed þ rx lnðrand1Þ ½cosð2p rand2Þ þ sinð2p rand2Þ.000 J/m3. / Applied Mathematical Modelling 30 (2006) 545–553 We assume that (rxij. for a very high density system.j which represent the cosines of the angle between the magnetic moment of the particle j. j¼1 r2xij þ r2yij þ r2zij 4.548 M. II ord. pﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃ ryij ¼ rymed þ ry lnðrand1Þ ½cosð2p rand2Þ þ sinð2p rand2Þ. and its anisotropy axis has a Gaussian distribution with variance ru generated by means of the Box–Mueller transformation: pﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃ ð21Þ uj ¼ ru lnðrand1Þ ½cosð2p rand2Þ þ sinð2p rand2Þ. ryij. for a high density system we can write ð24Þ f ¼ 0:32 f0 . rzij) are the components of the~ rij vectors that connect the center of i and j particles. l0 M 2s ð25Þ I ord. uj = cos h. 2. ryij. Numerical simulation method. r2ij ¼ r2xij þ r2yij þ r2zij . ryij and rzij. rz med. spontaneous magnetization Ms = 4. . 2). Osaci et al. We also assume that uj variables. pﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃ rzij ¼ rzmed þ rz lnðrand1Þ ½cosð2p rand2Þ þ sinð2p rand2Þ. ð18Þ ð19Þ ð20Þ rx. After the generation of these variables. by the average values rxmed. Using [3]. the HLi size for the i particle can be computed by using the following relation: n1 X d 3j ð3z2ij 1Þ ð22Þ H Li ¼ cd 3i qﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃ3 uj . rymed. and with most probable value of the particle diameter dm = 9. ð17Þ The rxij. III ord. ry and rz are the variances of the rxij.848 nm. Orders of the nearest neighbors for a very high density system. The particle’s ﬁrst-order neighbors for i particle. Fig.7 · 105 A/m. are the neighbors that are placed at one diameter distance from the central point of the i particle (Fig. results and model’s optimization The simulations were performed on a system with n = 270 spherical magnetite ﬁne particles with anisotropy constant K = 19. with f0 ¼ 8Kp . if we note with V powder f ¼ ð23Þ V test the volume fraction of particles. respectively.

In the ﬁrst approximation. II and III order and we use a parameter D — distance between two particles one next to each other (not between their central points).k = vr Æ rxmed. / Applied Mathematical Modelling 30 (2006) 545–553 549 Using (23)–(25). which corresponds to a concentration of the particles of 1.k = vr Æ rzmed. Osaci et al. we chose vr = 0. The ﬁrst order of the nearest neighbors for a diluted system.3 value.24 · 1023 part/m3.k. ð26Þ For the diluted systems. 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. ry.k the variance of the components rxij. rzij.k. For the simulations we are going to perform. we generally obtain the number of k order neighbors by using the following relation: 3 nk ¼ 0:32ð2k þ 1Þ f0 . we keep the number of neighbors of I. These calculations are performed under the hypothesis of weak or strong dipolar interaction.k. 2dm. which corresponds to a concentration of the particles of 2.M. the distance between the i particle and the nearest neighbors is 2dm. respectively. D 2d+D Fig. 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. rz. 4. 4dm to the next nearest neighbors. ryij. 4 and 5.k = vr Æ rymed. (2) weak interaction and (3) strong interaction. For a strong interaction. and 3dm. Fig.4 for the system of strong interactions. if the system of strong interactions is also studied. diﬀerent values of the parameter vr — Figs. which is bigger as the system is more diluted (see Fig. We note rx. rz.05. we considered that the particles are of the same diameter. 3.4 and diﬀerent values of the variance rx. ru = 0. 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. . and 6dm to the third-order particles. k being the order of the nearest neighbors for a given particle i.16 · 1024 part/m3 the distance between the i particle and the nearest neighbors is dm.k. ry. 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 ﬂuctuations with the number of particles from vr = 0.k. 3). In the weak interaction case.

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. For the generation of random values of particle diameters. (2) weak interaction and (3) strong interaction. . The method of generating a lognormal distribution is based on the relation d i ¼ erln d ui þln d 0 . Osaci et al. 6. Now. 6 that the variation of the distribution for the random variable uj = cos hj inﬂuences in a slight manner the average relaxation time.05. 5.550 M. It can be seen in Fig. we used the algorithm presented in [4–6]. Taking into account this estimated study. The distribution parameter of the distances between the particle i and the other particles in the system is ﬁxed to vr = 0. the simulations that follow will be done for the parameter vr = 0. 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. ð27Þ Fig.4.05 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. 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. we consider that particle dimensions have a lognormal distribution. / Applied Mathematical Modelling 30 (2006) 545–553 Fig.

. 7 shows the dependency of the average relaxation time on temperature. Fig. (10)–(12). Fig. In Eq. (2) with weak dipolar interaction and (3) with strong dipolar interaction. The dependency of the average relaxation time on temperature for the two kinds of interactions: (1) without dipolar interaction. (22) and the energy barriers of each particle by using Eqs. we ﬁrst generate the random variables. 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. 7. (27). 1). / Applied Mathematical Modelling 30 (2006) 545–553 551 where ui are the values of a normal distribution on (0. In the simulation algorithm. with the mean equal to ln d0 and the variance equal to r2ln d . Osaci et al. The average time relaxation analysis Fig. the time relaxations and the average time relaxation. Finally.848 nm corresponds to a volume of 5 · 1025 m3. 8. from Eq.M. (2) weak interaction and (3) strong interaction. (10). The most probable value of the particle diameter dm = 9. and then we computed the HLi size on the particles by using Eq. we have considered that the mean of the distribution is ln d0 = 18.4409 and the variance is r2ln d ¼ 0:01 ðrln d ¼ 0:1Þ. 5. which are used in the model.

7 that the average relaxation time for the ﬁne particle system decreases when the temperature increases. Dormann–Bessais–Fiorani and Morup–Tronc [1. . Finally we compared the simulated results to the model presented in this paper and also to the models from the literature: Ne´el–Brown. it may be seen that the average relaxation time increases with the growth of the dispersion of the random variable. From Figs. Osaci et al. Fig. 8–10 show the dependency of the average relaxation time on the logarithm of the variance of the particle diameters for 100. 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. In these ﬁgures vr = 0.7] — Fig. 8 to 10. 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.4.05 and ru = 0.65 the resulted values obtained by using the model presented in this paper are situated between the resulted values obtained by Dormann–Bessais–Fiorani and Morup–Tronc models. Figs. 10.1. In Fig.552 M. / Applied Mathematical Modelling 30 (2006) 545–553 It is shown in Fig. 150 and 200 neighbor particles at 300 K. 11. it can seen that below r = Kv/kBT = 2. 11 for ﬁne magnetite particles at 300 K with rln d = 0. 9. (2) weak interaction and (3) strong interaction. Fig.

Bucharest.M. van Heereden.F. H. Ermakov. S. Koch. Swart. It is observed in Figs. on the natural logarithm variance of diameters and on the particle volume. 6. Academy Publishing. The Random Numbers.G. 36–57. References [1] [2] [3] [4] [5] M. there can be observed an inﬂuence for the dependency between average relaxation time and the temperature. I. there has been proposed a 3D model. / Applied Mathematical Modelling 30 (2006) 545–553 553 Fig. [7] L.H. 6–8 that the average relaxation time is inﬂuenced by the dipolar interaction strength and also by the natural logarithm variance of particle diameter. The increase is less signiﬁcant when the dipolar magnetic interaction is strong. It has been also considered that hj angles are random Gaussian variables. Technique Publishing. Porto. with a Gaussian distribution generated by means of the Box–Mueller relation. Hansen. 11. 36–57. P. Rivas. Journal of Magnetism and Magnetic Materials 184 (1998) 262–274. IEEE Transactions on Power Delivery (1995) 1733–1740. Considering the dipolar magnetic interaction between particles. Morup. pp. A. J. Ne´el. similar to a real situation. R. Based on Dorman–Bessais–Fiorani model [1]. 1994. Petersen. Garcia-Otero. J. with Dormann–Bessais–Fiorani model (1) and with Ne´el–Brown model (4). . Industry and in the Study of Natural Phenomenon. Annales de Geophysique 5 (2) (1949) 99–136. Monte Carlo Method and Connected Problems. Cluj-Napoca. D. pp. Physical Review Letters 84 (1) (2000) 167–170. [6] I.M. 43–47. Mihoc. S. Bunde. Bucharest. 1978. Sa˘cuiu. Babes-Bolyai University Publishing. The dependency between s/s0 and Kv/kBT with present model (2). with Morup–Tronc model (3). In this model it has been considered that the particles are randomly arranged in a volume.M. Conclusions In this paper a simulation has been carried out to determine the dependency of the average relaxation time for a ﬁne particle system on the temperature. pp. 1976. Zorilescu. R. Calculus of Probability and Mathematical Statistics. Applications in Economy. It results in an increase of the average relaxation time by temperature’s decreasing. Osaci et al. M.

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