Journal of Magnetism and Magnetic Materials 368 (2014) 240–245

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Journal of Magnetism and Magnetic Materials

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

Studies of superspin glass state and AC-losses in La0.7Sr0.3MnO3

nanoparticles obtained by high-energy ball-milling
P.T. Phong a,b,n, D.H. Manh c, L.H. Nguyen b,c, D.K. Tung c, N.X. Phuc b,nn, I.-J. Lee a,nnn
a
Department of Advanced Materials Chemistry, Dongguk University-Gyeongju, 707 Suckjang-dong, Gyeongbuk, Gyeongju-Si 780-714, Korea
b
Nha Trang Pedagogic College, 1 Nguyen Chanh Street, Khanh Hoa Province, Nha Trang City, Viet Nam
c
Institute of Materials Science, Vietnam Academy of Science and Technology, 18 Hoang Quoc Viet Road, Cau Giay District, Ha Noi City, Viet Nam

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

Article history: Single-phase perovskite compound La0.7Sr0.3MnO3 was synthesized by a high-energy ball milling
Received 28 October 2013 method. Nanoparticle nature of this manganite with the average particle diameter of 11 nm was
Received in revised form revealed from structure and morphology characterizations. The results of ac magnetic susceptibility
11 April 2014
measurements show that the system can be described as an ensemble of interacting magnetic
Available online 24 May 2014
nanoparticles, which indicates that the dipole–dipole interactions are strong enough to create superspin
Keywords: glass state in the sample. Furthermore, the specific loss power which is exhausted on the irradiation of
La0.7Sr0.3MnO3 an ensemble of particles with a magnetic field has been calculated and measured experimentally.
Superspin glass & 2014 Elsevier B.V. All rights reserved.
AC-losses
Nanoparticle

1. Introduction nanoparticle has large magnetic moment (the so-called superspin)

Over the past decades, perovskite manganites of the type
R1
xMxMnO3 (where R¼Rare earth ions, and M ¼Alkaline ions)
have attracted attention due to their interesting physical proper-
ties such as colossal magnetoresistance (CMR), magnetocaloric
effect, charge ordering, orbital ordering, and spin ordering [1–3].
Most of the previous studies on R1
xMxMnO3 focused on proto-
typical compound with x near 0.33, which exhibits an optimal for
the occurrence of both ferromagnetism and metallic conductiv-
ities. Among them, one of the most studied compounds is
La0.7Sr0.3MnO3 [4,5], which has high magnetic ordering tempera-
ture (365 K) as well as fully stable FM phase. Since the recent
discovery of low field magnetoresistance (LFMR), many studies
have shown that grain size, especially nanometer scale, plays an
important role in numbers of unique properties in these materials,
such as LFMR, low saturation magnetization, surface spin-glass
and superparamagnetic behavior. In nanomaterials, most physical
properties strongly depend on their size, shape, size distribution
and interaction between the particles [6–8]. If the particle size is
smaller than the size of a single domain, each ferromagnetic
n
Corresponding author at: Department of Nanomaterial Chemistry,
Dongguk University-Gyeongju, Korea.
nn
Correspondence to: Institute of Materials Science, Vietnam Academy of Science
and Technology, Viet Nam. Tel.: þ 84 43756 4129; fax: þ 84 43836 0705.
nnn
Correspondence to: Department of Nanomaterial Chemistry, Dongguk
University-Gyeongju, Korea. Tel.: þ 82 54 770 2220; fax: þ82 54 770 2386.
E-mail addresses: ptphong.nh@khanhhoa.edu.vn (P.T. Phong),
phucnx1949@gmail.com (N.X. Phuc), lij@dongguk.ac.kr (I.-J. Lee).
[9–12]. According to the particle size effect and the interactions
between superspins, magnetic behavior of the material is classi-
fied into two types, superparamagnetic (SPM) and superspin glass
(SSG). The noninteracting superspins give rise to superparamag-
netic behavior. In the SPM state, each particle thermally fluctuates
between its easy directions of magnetization and freezes along
these directions at the blocking temperature (TB), where the
relaxation time τ becomes equal to the measuring time τm. The
relaxation time is typically described by the Néel–Arrhenius law.
The SPM behavior was predicted at high temperature and the
blocked state at low temperature [11,13]. When the interactions
between the superspins become sufficiently strong, the interacting
superspins cause the superspin glass behavior below a freezing
temperature (Tf) [11]. In this case, the interaction behavior of
system can be taken into account in the Vogel–Fulcher law, which
is a modification of the Néel–Arrhenius law [8–14]. Moreover, in
some cases, the critical slowing down law, which assumes the
existence of true equilibrium phase transition with a divergence of
relaxation time near the transition temperature, has been used to
search the relaxation behavior in superspin glass and spin-glass
systems [11,14]. Generally, it is well known that ac magnetic
susceptibility is one of the useful techniques to distinguish
between SPM and SSG systems. This technique is used to
study the dynamics of magnetic properties of magnetic nanopar-
ticles [15,16].
In recent years, some physical properties of nanoparticle
La0.7Sr0.3MnO3 (LSMO) manganites were studied in few papers
[17–23]. Rostamnejadi et al. [17,21] have prepared single phase
LSMO nanoparticles by the sol–gel process and investigated their

http://dx.doi.org/10.1016/j.jmmm.2014.05.025
0304-8853/& 2014 Elsevier B.V. All rights reserved.
 P.T. Phong et al. / Journal of Magnetism and Magnetic Materials 368 (2014) 240–245
structural and magnetic properties. Magnetic dynamics of the
samples was studied by the measurement of ac magnetic suscept-
ibility vs. temperature at different frequencies and ac magnetic
fields. A frequency dependent peak was observed in ac magnetic
susceptibility vs. temperature which is well described by Vogel–
Fulcher and critical slowing down laws. They found that in this
system, there is strong interaction between magnetic nanoparti-
cles and its magnetic behavior is superparamgnetic. Dyakonov
et al. [18] have studied magnetic, resonance and transport proper-
ties of LSMO nanopowders in detail and shown that both Curie
temperature and magnetization decrease with decrease in the
particle size. They believed that the decrease of magnetization and
other intrinsic parameters of the nanoparticles have their origin in
surface effects. Muthuselvam and Bhowmik [22] have studied
magnetization, ac susceptibility, resistivity and magnetoresistance
in mechanically milled LSMO. In their report, the samples are
typical soft ferromagnet that transformed from multi-domain
state to single domain state in nanocrystalline samples. Further-
more, they have observed that low temperature freezing of
ferromagnetic domains/clusters does not follow the conventional
spin glass features. To our best knowledge, however, the
researches on the superspin glass characteristics of LSMO manga-
nite nanopowders have not been systematically investigated so far.
In particular, for hyperthermia application for tumor therapy, it is
necessary to have fairly uniform particle size and a Curie tem-
perature above room temperature. However, although there are
numerous empirical results on magnetic hyperthermia, none of
them systematically explains why the published data on the AC
losses in magnetic nanoparticles are widely scattered as well as
what the mechanism of the losses is [24,25]. Also, there is little
data on the relation of the ac losses to the magnetic parameters of
a separate nanoparticle and its size [26].
In this paper, we have studied the magnetic properties and ac
losses of LSMO nanoparticles. The ac magnetic susceptibility vs.
temperature at different frequencies, zero-field-cooled (ZFC) and
field-cool (FC) magnetizations has been performed to investigate
the magnetic dynamic of magnetic LSMO nanoparticles. The Néel–
Arrhenius, Vogel–Fulcher, and critical slowing down models have
been used to study the dynamical properties. The decrease in FC
magnetizations at low temperatures was clearly observed in LSMO
nanoparticles and this result indicates that the SSG phase occurs
below a spin freezing temperature. Furthermore, the H–T diagrams
are studied using the temperature dependence of ZFC of LSMO
nanoparticles at various H. The peak temperatures of the ZFC
magnetizations of this system are determined as a function of H.
We observed that the ZFC-peak temperature Tp (¼ Tf) for LSMO
nanoparticles decreases with increasing H, forming a critical line
with an exponent p equal to the de Almeida–Thouless (AT)
exponent (¼3/2) [27]. This critical line is the phase boundary
between the SPM and SSG phases. These results can be well
described by the SSG model of strong magnetic dipole interaction
between LSMO nanoparticles. Moreover, based on the linear
response theory using the Neel–Brown relaxation time, the spe-
cific loss power for LSMO nanoparticles was also calculated and
discussed in detail.
2. Experimental
Nanocrystalline samples of La0.7Sr0.3MnO3 were synthesized
by a high-energy ball-milling method. La2O3, SrCO3 and MnO2
powders with 99.9% purity from Merck were used as starting
materials. The details of fabrication conditions were thoroughly
described in a previous report [28]. The average grain sizes
and grain size distributions of the nanosystem were determined
using a commercial WIN-CRYSIZE program packet based on the
241
Warren–Averbach formalism [29]. After only 8 h of milling, single
phase sample with grain size of 11 nm was obtained, whereas the
morphology of grains obtained from TEM is spherical or nearly
spherical with the grain size of 17 nm [28]. All magnetic measure-
ments were carried out using Quantum Design Physical Property
Measurement System (PPMS). Three different types of measure-
ments have been used for the study of the following magnetic
properties: frequency and temperature dependence of AC suscept-
ibility χ(ν, T), temperature dependence of DC magnetization M(T)
in the FC and ZFC modes, and magnetic field of isothermal
magnetization M(H) at various temperatures. In order to deter-
mine specific loss power (SLP) of the ferrofluids synthesized
nanoparticles were prepared by dispersing 5 mg LSMO in 1 ml of
deionized distilled water and placed into a coil that provides the
alternating magnetic field (frequency 236 kHz, amplitudes up to
80 Oe). The SLP was calculated using the following expression
[30]:
ms dT
SLP ¼ C ð1Þ
mi dt
where C and ms are, respectively, the heat capacity and mass of the
ferrofluid, mi is the mass of magnetic LSMO nanoparticles, and
dT/dt is the initial slope of the heating curve.
3. Results and discussion
Fig. 1 shows the temperature dependence of the ZFC and FC
magnetization (M–T curves) for LSMO under applied field of 10 Oe.
In the ZFC mode, the magnetization increases at first, and then
decreases with increasing temperature. The MZFC–T curve exhibits
a peak at 236 K followed by a broadened ferromagnetic to
paramagnetic transition. A typical peak in the ZFC curve is found
in both SPM and SSG samples [31]; however, the decrease in
MFC(T) indicated in the inset of Fig. 1 can only be observed in SSG
systems [32]. The dip is due to an additional PM signal from small
clusters or atoms dispersed between the particles [33]. This fact
implies the formation of ferromagnetic clusters with a SSG state in
our sample. The SSG behavior will be discussed later in detail.
In addition, a large separation between MFC(T) and MZFC(T) curves
below the irreversibility temperature is also observed. This is
assigned to the presence of a strong magnetic anisotropy. The
gap between MFC(T) and MZFC(T) would change depending on the
homogeneity in magnetism of sample and on the magnitude of
applied field. The samples exhibit not only ferromagnetic (FM) and
antiferromagnetic (AFM) interaction but also magnetic frustration
(i.e., there is a strong competition between FM and AFM
0.7
0.6 0.67
ZFC
FC
M (emu/g)
0.5
M (emu/g)
0.4
0.66
0 20 40 60 80 100
0.3
T (K)
0.2
0.1 H = 10 Oe
0
0 50 100 150 200 250 300 350
T (K)
Fig. 1. Temperature dependence of ZFC–FC magnetization of the nanosized
La0.7Sr0.3MnO3. Detail of MFC vs. T at low T is shown in the inset.
242 P.T. Phong et al. / Journal of Magnetism and Magnetic Materials 368 (2014) 240–245

interactions) usually display wide gap [34–38]. The FM–PM phase-
transition temperature (TC) obtained from the minimum of the
dMZFC/dT curve is about 307 K (its dMZFC/dT
T curves are not
shown), which is much smaller than that of a bulk sample (with
TC ¼365 K). Here, the decrease in the FM–PM phase-transition
temperature is due to the cleavage of Mn–O–Mn bonds at the
surface of nanoparticles, which hampers exchange interaction
[39].
Fig. 2, plots χ ¼ (M/H)
1 vs. temperature, exhibits a well-
defined Curie–Weiss behavior χ(T) ¼C/(T
θ) (red line in the
figure) with a Curie–Weiss constant C ¼11.87  10
3 emu K/Oe g
and Curie–Weiss temperature θ ¼320 K. The θ value is higher than
TC (307 K), which is assigned to the presence of FM–spin interac-
tions above TC [36]. From this fit the effective paramagnetic
moment was calculated using expression [40]
N A μ2B 2
C¼ μ ð2Þ
3kB eff
where NA ¼6.023  1023 mol
1 is the Avogadro number, μB ¼9.274 
10
21 emu is the Bohr magneton and kB ¼1.38  10
16 erg K
1 is
the Boltzmann constant. The effective magnetic moment ðμeff Þ of
4.64μB is determined. On the other hand, μeff of La30:7þ Sr20:3þ
Mn30:7þ Mn40:3þ O23
can be written as
μ2eff ¼ ð1
xÞμ2eff ðMn3 þ Þ þ xμ2eff ðMn4 þ Þ
where μeff is obtained from experimental (4.64μB), μeff ðMn
4:90μB and μeff ðMn4 þ Þ ¼ 3:87μB . The obtained value of x¼0.28
shows that Mn4 þ /Mn3 þ ratio is similar to Sr2 þ /La3 þ giving good
600
500
400
(Oe.g/emu)
stoichiometry with the small excess of oxygen of δ ¼0.02 which is
within the experimental error.
As mentioned above, the magnetic measurements indicate that
LSMO exhibits SSG behavior. To explore the origin of the SSG
properties, we have also measured ac susceptibility at the field of
H¼ 1 Oe and at several different frequencies and its results are
presented in Fig. 3(a) and (b). Both χ 0 and χ 00 were measured at
several frequencies between 33 and 1089 Hz in the temperature
range 50–300 K. It shows that the real part of ac magnetic
susceptibility appears as a broad peak while imaginary part as a
relatively sharp peak. The peak of χ 0 shifts to the higher tempera-
ture side with increasing frequency. For example, the peak is
213.9 K (T p ðχ 0 Þ) for f ¼33 Hz while 223.4 K for f ¼1089 Hz. Also, the
peak high of χ 0 increases with decreasing frequency. Similar to χ 0 ,
the peak of χ 00 also shifts to the higher temperature side with
increasing frequency, for instance, T p ðχ 0 Þ ¼225.5 K for f¼ 33 Hz
while T p ðχ 0 Þ ¼ 262.5 K for f ¼1089 Hz. And its peak height of χ 00
decreases with increasing f.
It is known that the empirical criterion parameter c defined by
c ¼ ð1=T p ÞΔT p =Δðlog 10 ωÞ ð4Þ
is one of the important parameters that distinguishes spin glasses
(co 0.06) from superparamagnets (cE 0.3). Here c is estimated as
0.03, which implies that our system is not a SPM but a SSG.
ð3Þ According to Hansen et al. [42], there are two criteria to determine
the freezing temperature. One is the freezing temperature defined
3þ
Þ¼
as the temperature at which χ 00 attains 15% of its maximum value.
The other is the freezing temperature defined from the relation
χ 0 ðω; T f Þ ¼ 0:98χ FC ðT ¼ T f Þ. According to Suzuki et al. [11], however,
we adopt here the freezing temperature (Tf) as the peak tempera-
ture T p ðχ 0 Þ for convenience.
In order to investigate the magnetic dynamics, we have applied
three different models to our sample. For a system consisting of
non-interacting superparamagnetic (SPM) particles, the relaxation
time is given by the Neel–Arrhenius (NA) mode [43],

300 lnðf Þ ¼ lnðf 0 Þ
Ea =kB T ð5Þ

where Ea is the activation energy, kB is the Boltzmann constant,

-1

200
and T is the temperature. Fig. 4 shows that the experimental data
fit well into Eq. (5). When the data are fitted to the NA model, f0
100 and Ea/kB are estimated as 7.46  1035 Hz and 16844 K, respec-
tively. f0, about 1036 Hz, is very large compared to the generally
0 accepted Larmor frequency of 109–1013 Hz and, therefore, it seems
0 50 100 150 200 250 300 350 400 to be physically unrealistic [43]. The result implies that the
T (K) nanoparticles are not independent and there exists interaction
Fig. 2. Inverse susceptibility vs. temperature of LSMO obtained from magnetization between them. For weakly interacting magnetic nanoparticles, the
measurement in a field of 10 Oe. (For interpretation of the references to color in frequency dependence of Tf is given by the Vogel–Fulcher (VF) law
this figure, the reader is referred to the web version of this article.) [44]; the VF model is a modification of the NA model which

0.045 0.0012

0.04 0.001

0.035 0.0008
'' (emu/g)
' (emu/g)

33 Hz 33 Hz
0.03 99 Hz 0.0006 99 Hz
198 Hz 198 Hz
0.025 396 Hz 0.0004 396 Hz
594 Hz 594 Hz
0.02 792 Hz 0.0002 792 Hz
1089 Hz 1089 Hz
0.015 0
50 100 150 200 250 300 50 100 150 200 250 300
T (K) T (K)
Fig. 3. Real (a) and imaginary (b) parts of ac susceptibility for LSMO sample vs. temperature in frequencies of 33–1089 Hz and ac field of 1 Oe.
 P.T. Phong et al. / Journal of Magnetism and Magnetic Materials 368 (2014) 240–245 243

ordering and zν is the dynamical exponent [7,41,46,47]. This

7 equation fits our experimental data excellently and is displayed
in Fig. 6. The fitting parameters of τ0, Tg and zν are 6.28  10
12 s,
ln(f)
223 K and 7.2, respectively. These results suggest the existence of
6
the SSG behavior in the sample, which are consistent with the
result of dc magnetization.
The phase transition of a SSG system was described using the
ln(f)

5
mean-field picture based on the Edwards–Anderson (EA) model
[48]. In the presence of a magnetic field the phase boundary
4 between the SPM phase and the SSG phase has been predicted by
the Almeida and Thouless (AT) line [27], and can be written as
  p 
3 H
T ¼ Tf 1
ð8Þ
Ha
212 214 216 218 220 222 224
T f (K) where Tf is freezing temperature at H ¼0, Ha ¼2Keff/ρMS is aniso-
tropy field, Keff is effective anisotropy constant, MS saturation
Fig. 4. Plot of Tf against ln(f) for LSMO sample. The solid lines indicate the best fit of magnetization and ρ being density of the sample. The exponent
ln(f) vs. Tp for the samples by using Néel–Arrhenius law.
p depends on the interaction strength. In noninteracting systems,
p¼ 2 [49] while for interacting case this parameter is close to 2/3
[50]. Fig. 7 shows the temperature dependence of MZFC for LSMO
nanoparticles at various external fields (H). The peak temperature
7
Tp decreases with increasing H. The least-squares fit of the data
ln(f)
(open symbols) and solid line in Fig. 8 to Eq. (8) yield the
6 parameters Tf ¼234 K and Ha ¼ 1348 Oe. These results indicate that
there is an AT critical line in the H–T phase diagram for LSMO
nanoparticles as a SSG system. We believed that the nature of the
ln(f)

5 AT line in SSG systems is essentially the same as that in the SG

systems. Using density of the LSMO sample, ρ ¼5.98 g/cm3 [51],

4
0.006

3 0.005

212 214 216 218 220 222 224 0.004

T f (K)
(s)

0.003
Fig. 5. Plot of Tf against ln(f) for LSMO sample. The solid lines indicate the best fit of
ln(f) vs. Tf for the sample by using Vogel–Fulcher law.
0.002

0.001
includes the addition of another term, T0 (T0 is an effective
temperature which represents the existence of the interaction
0
between nanoparticles), which describes the energy scale of the 212 214 216 218 220 222 224
dipolar interactions and is expressed as
T (K)
f
lnðf Þ ¼ lnðf 0 Þ
Ea =kB ðT
T 0 Þ ð6Þ
Fig. 6. Plots of τ vs. Tf for the LSMO sample with the best fitted lines using
In Fig. 5 we have fitted the experimental data of real part in our conventional critical slowing down law.
samples by using Eq. (6). The estimated values of f0, Ea/kB and T0
from this fitting are 3.7  104 Hz, 67 K and 205 K, respectively. 25
As pointed out, f0 (104 Hz) are at least four orders of magnitude
10 Oe
smaller than that of the typical value of f0  108–1011 Hz for weakly
20 50 Oe
interacting nanoparticles [44]. This may indicate that there is
strong dipole–dipole interaction in agglomerated LSMO nanopar- 100 Oe
ticles [45]. Therefore, we believe that the presence of strong 250 Oe
15
M (emu/g)

dipole–dipole interaction in our case causes a strong interaction 500 Oe

between these LSMO nanoparticles. The increase in dipole–dipole
interaction could create the SSG behavior in nanoparticles 10
of LSMO.
It is well known that the frequency dependence in the SSG
5
system can be described as
 
zν
T
τ ¼ τ0
1 ð7Þ 0
Tg 50 100 150 200 250 300 350
where τ is the characteristic relaxation time of the system being T (K)
probed by the ac frequency, τ0 is the relaxation time of the Fig. 7. Temperature dependence of ZFC magnetization of nanosized LSMO in
individual particle moment, Tg is the critical temperature of SSG different magnetic fields.
244 P.T. Phong et al. / Journal of Magnetism and Magnetic Materials 368 (2014) 240–245

240
as [54]
     
μH μH kB T
220 M ¼ nμL þ χ H ¼ nμ coth
þ χH ð10Þ
Tp kB T kB T μH
200
In Fig. 9 we plotted the M(H) curves for the LSMO nanoparticles
180 at T¼ 10 K and 300 K. There is a huge reduction of the magnetization
T p (K)

compared to the theoretical value. Such a drastic decrease of the

160
magnetization could be explained by considering the large surface-
140 to-volume ratio in nanoparticles. Red lines and black lines in this
figure present the results of the fitting of experimental data with
120
Eqs. (9) and (10), respectively. As can seen in Fig. 9, the application of
100 Eq. (9) to the M(H) curves is inconsistent with the experimental
data. Contrary, we can see that Eq. (10) well explains the experi-
0 10 20 30 40 50 60 70
mental data, which makes it possible to calculate the magnetic
H2/3 (Oe2/3) moment of a single superparamagnetic particle, μ ¼ 91.69  102μB
Fig. 8. Plot of Tp as a function of H2/3 for LSMO nanoparticles. The solid line is least- (where μB is the Bohr magneton), and particle concentration
squares fitting curve to Eq. (8). n¼ 5.20  1017 cm
3. Thus, one magnetic particle occupies a volume
of 1.94  10
18 cm3, which corresponds to the particle diameter
d¼ 15.4 nm.
The ac losses for the LSMO nanoparticles placed in an external
50 electromagnetic field were calculated using the two types of
relaxation process, namely Neel and Brown relaxations. According
to Carrey et al. [55], linear response theory can be used for
40
describing the response of an assembly of magnetic nanoparticles
10 K
using the Neel–Brown relaxation time with the assumption that
10 K
30 the magnetic system responds linearly to the magnetic field. This
M (emu/g)

300 K
model is suitable for calculation of ac-losses in superparamagnetic
300 K nanoparticles at low magnetic field [56]. Under this assumption,
20 the power loss for superparamagnetic nanoparticles is given by

2π 2 f τ
2

10
Pðf ; HÞ ¼ μ0 χ H 20 ð11Þ
1 þ ð2π f τÞ
2

where μ0 ¼4π  10
7 T mA
1 is the vacuum susceptibility, χ is the

0 magnetic susceptibility of the powder, H0 is the intensity of
0 10 20 30 40 50
magnetic field, and f is the frequency of electromagnetic field.
H (kOe)
In case the ensemble of superparamagnetic particles magnetic
Fig. 9. M–H data of LSMO sample measured at 10 K and 300 K. Red line curves moment μ, magnetic susceptibility χ can be calculated using
fitted with Eq. (9) and black line curves fitted with Eq. (10). (For interpretation of
formula [10]:
the references to color in this figure legend, the reader is referred to the web
version of this article.)
μ0 μ2
χ ¼n ð12Þ
3kB T

and taking MS ¼46.7 emu/g obtained from M(H) measurement at
10 K (see later Fig. 9) and Ha ¼2Keff/ρMS, effective anisotropy
constant of Keff ¼ 1.9  105 erg/cm3 is obtained which is one order
of magnitude larger than that in similar nanoparticles manganite
[52]. This difference may be due to other sources of magnetic
anisotropies like shape anisotropy and surface anisotropy or
magnetic interaction between nanoparticles [17]. However, this
value is close to that of La0.7Ca0.3MnO3 prepared by high-energy
ball milling of Spasojevic et al. [14]
In the coming section, in order to quantitatively understand the
nature of M–H curve at 10 K and 300 K, we have used the
framework of theory of the superparnmagnetic initiated by
Langevin to analyze the obtained data. In superparamagnetic
regime, the temperature and field dependence of magnetization
of an assembly of noninteracting particles with uniform size is
given by Langevin relation [53]
     
μH μH kB T
M ¼ nμL ¼ nμ coth
ð9Þ
kB T kB T μH
where L is Langevin function, n is concentration of particles and kB
is the Boltzmann constant.
In case if there is small fraction of paramagnetic fraction
in addition to superparamagnetic particles, Eq. (9) can be written
The relaxation time can be written in the form [55]:
K eff V
τ ¼ τ0 exp ð13Þ
kB T
where τ0 ¼ 10
9 s [57].
The SLP was calculated for the LSMO nanopowder placed in
electromagnetic field with f ¼236 kHz and H0 ¼80 Oe. Magnetic
susceptibility, χ 00 , calculated for the LSMO powder using Eqs. (10)
and (12), is 15.14  10
3 emu Oe
1 g
1. As a result, P ¼3.30 W/g,
which is somehow lower than that estimated experimentally for
the LSMO nanopowder is synthesized in this study, namely,
Pexp ¼5.32 W/g for the measurement with field of f¼ 236 kHz
and H0 ¼80 Oe. One needs more studies for carrying detail
discussion about the low and/or the difference in estimated values
of P, but from the TEM image [28] and the above discussions we
believe to exist an influence of the strong interaction between the
LSMO nanoparticles at 300 K [58].
As it can be seen from Eqs. (12) and (13), the SLP is very
sensitive to the particle volume. So, the increase in V gives rise to
the increase in both magnetic susceptibility χ and relaxation time
τ, which is expected to lead to a significant enhancement of P. It is
worth noting that Yelenich et al. [56] have also recently calculated
the ac-losses in NiFe2O4 nanoparticles. They found that these data
agree well with the experimental results.
 P.T. Phong et al. / Journal of Magnetism and Magnetic Materials 368 (2014) 240–245 245

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