Theoretical investigation on the magnetocaloric effect in garnets R 3 Fe 5 O 12 where (

R = Y and Dy)
P. J. von Ranke, B. P. Alho, E. J. R. Plaza, A. Magnus G. Carvalho, V. S. R. de Sousa, and N. A. de Oliveira
Citation: Journal of Applied Physics 106, 053914 (2009); doi: 10.1063/1.3213383
View online: http://dx.doi.org/10.1063/1.3213383
View Table of Contents: http://scitation.aip.org/content/aip/journal/jap/106/5?ver=pdfcov
Published by the AIP Publishing
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JOURNAL OF APPLIED PHYSICS 106, 053914 2009

Theoretical investigation on the magnetocaloric effect in garnets R3Fe5O12

where R = Y and Dy
P. J. von Ranke,1,a B. P. Alho,1 E. J. R. Plaza,1 A. Magnus G. Carvalho,2
V. S. R. de Sousa,1 and N. A. de Oliveira1
1

Instituto de Fsica Armando Dias Tavares, Universidade do Estado do Rio de Janeiro (UERJ), Rua So
Francisco Xavier 524, 20550-013 Rio de Janeiro, Brazil
2
Diviso de Metrologia de Materiais, Instituto Nacional de Metrologia, Normalizao e Qualidade
Industrial, Duque de Caxias, 20550-013 Rio de Janeiro, Brazil

Received 6 May 2009; accepted 7 August 2009; published online 15 September 2009
In this work the magnetocaloric effect in ferrimagnetic rare-earth iron garnets R3Fe5O12 where R
= Y and Dy was theoretically investigated considering a model Hamiltonian, which takes into
account three coupled magnetic sublattices in the mean field approximation. In Dy3Fe5O12 the
inverse magnetocaloric effect was predicted and associated with the compensation temperature. Our
theoretical results for the adiabatic temperature change in both compounds are in good agreement
with the experimental data. 2009 American Institute of Physics. doi:10.1063/1.3213383
I. INTRODUCTION

In the past 12 years much effort has been concentrated in

the investigation of the magnetocaloric effect MCE, which
is basically measured by the adiabatic temperature change
and the isothermic entropy change upon magnetic field
changes. The MCE was discovered in 1881 by Warburg,1 and
the more recent interest was due to the discovery of the first
giant MCE around room temperature in Gd5Si2Ge2 in 1997
by Pecharsky and Gschneidner.2 The magnetic materials,
which produce a large MCE, especially around room temperature, are desired in order to be used in magnetic refrigeration process, which is preferable from the environmental
point of view, since no volatile liquid refrigerants that have a
negative influence on Earths atmosphere are used.35 Besides the technological interest, the study of the MCE has
fundamental importance in order to understand the basic
physical properties of magnetic materials, e.g., the coupling
between magnetic lattice and crystalline lattice,6 the nature
of the first and second order magnetic phase transitions,7,8
the crystalline electrical field CEF and magnetic
anisotropy,9,10 the charge-ordering contribution to the entropy change,11,12 and the magnetic disorder problems.13,14
In this work we report the theoretical investigation on
the MCE in the rare-earth iron garnets, which are described
by the chemical unit formula R3Fe5O12. The Fe ions are localized in two different crystallographic sites. Two Fe ions
occupy the octahedral sites and three Fe ions occupy the
tetrahedral sites formed by the nearest oxygen ions. The
three R ions in our case R = Y or Dy are surrounded by
eight oxygen ions located at the corners of a skewed cube,
which is often called dodecahedron sites. These three crystallographic sites are properly labeled by the following letters derived from crystallographic notation: c dodecahedral
sites, d tetrahedral sites, and a octahedral sites. The gar-

nets are nonconductors and the magnetic interactions among

the magnetic ions are intermediated by the oxygen atoms, the
so-called superexchange interaction. Due to the structural
crystallographic parameters15 it is expected that the c- and
d-sublattices exchange interactions would be smaller than
that between a- and d-sublattices. Also, the magnetic moment in the a-d couplings is antiparallel as confirmed16,17 by
neutron diffraction experiments in Y3Fe5O12. Besides, it was
observed experimentally that independent of the rare-earth
ion in the c site, the Nel temperature of the garnets is relatively constant, indicating that a and d sites Fe antiferromagnetic interaction is the dominant one. This condition will
be exploited in order to simplify our calculation.
II. THEORY

In our model the magnetic lattice of R3Fe5O12 is formed

by three magnetic sublattices in the presence of an external
magnetic field. The Hamiltonian for this system is given by
i,j a d
i,j a c
i,j d c
H = ad
Ji J j ac
Ji J j dc
Ji J j
i,j

i,j

i,j q q
qq
Ji J j BB gqJqi ,

i,q
i,j,q

where the first three terms are the intersublattices exchange

interactions, whose intensities are given by the exchange pai,j
i,j
i,j
rameters ad
, ac
, and dc
. The last two terms are the
intrasublattices exchange interactions and the Zeeman interaction q = a, d, c runs over the three sublattices, B is the
external magnetic field, gq is the Land factor, and Jq represent the total angular momentum operators of the magnetic
ions in the sublattices. Extracting from Eq. 1 the single ion
Hamiltonian in molecular field approximation, we have
H = adZadJaJd adZdaJdJa acZacJaJc

Author to whom correspondence should be addressed. Also at Dep. de

Eletrnica Quntica, Instituto de Fsica, Universidade do Estado do Rio de
Janeiro, Rua So Francisco Xavier, 524-3 andar., Maracan, Rio de Janeiro 20550-013, Brazil. Electronic mail: von.ranke@uol.com.br.

0021-8979/2009/1065/053914/6/$25.00

i,j

106, 053914-1

acZcaJcJa + dcZdcJdJc dcZcdJcJd

qqZqqJqJq BB gqJq ,
q

2009 American Institute of Physics

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053914-2

J. Appl. Phys. 106, 053914 2009

von Ranke et al.

where Zad is the number of nearest magnetic ions neighbors

with total angular momentum Jd of the magnetic ion with
total angular momentum Ja, and so on for the others
Z-numbers. The Jq is the thermodynamic mean value of the
total angular momentum in the q-sublattice and is directly
related with the sublattice magnetization
M q = NqBgqJq.

Here, Nq is the number of magnetic ions per magnetic sublattice; i.e., Na = 2 and Nd = Nc = 3.
Hamiltonian 2 can be written in the simplified form
H = Bg aB aJ a Bg dB dJ d Bg cB cJ c ,

fect with an effective gc factor, that is, gc gc cos instead of the procedure presented by Dionne,19 in which was
proposed Jc Jc cos . In fact, the quenching due to the
CEF reduces the magnetic moment without changing the
number of the magnetic quantum states 2Jc + 1, and consequently not changing the maximum magnetic entropy, as will
be discussed below.
The magnetic entropy change S versus T in an isothermic process that occurs for magnetic field change B : 0
B0 can be calculated by the integration of Maxwell relation
S =

where
5

Bd = B + adM a + ddM d + dcM c ,

6
7

and aa, dd, cc, ad, ac, and dc are the normalized effective exchange interaction parameters. Using Hamiltonian 4,
the mean values Jq can be calculated leading to the three
coupled magnetic state equations
M a = NagaBJaBJagaBJaBa/kT,

B0

Ba = B + aaM a + adM d + acM c ,

Bc = B + acM a + dcM d + ccM c ,

M d = NdgdBJdBJdgdBJdBd/kT,

M c = NcgcBJcBJcgcBJcBc/kT,

10

where BJqx is the Brillouin function; Ja, Jd, and Jc are the
total angular momentum number Ja = Jd = 5 / 2 for Fe ion,
Jc = 15/ 2 for Dy ion, and Jc = 0 for Y ion; B is the Bohr
magneton; and k is the Boltzmann constant.
The contribution of the orbital Lq and the spin Sq angular
momenta to the effective magnetic momentum at T = 0 K
due to the magnetic ion in the q-sublattice would be gqJqB.
For q = a, d we have Fe ions and only the spin contribution
exists, so ga = gd = 2 and Ja = Jd = Sa = Sd = 5 / 2. Depending on
the rare-earth ions in the c-sublattice the orbital angular momentum should be considered and the expected total spontaneous magnetic moment at T = 0 K is M 0 = 3gcJc + 2gaSa
3gdSdB / f.u., since the rare-earth ions couple antiparallel
to the resultant Fe-sublattices magnetic moment. Nevertheless, for rare-earth garnets, the observed moments generally
. The explanalie below the expected values M 0 M expected
0
tion is that the orbital momentum is partly quenched and
nonantiparallel arrangement between the magnetic moments
in the c- and a-d-sublattices due to the CEF effect occurs.18
In our model we do not consider the CEF interaction in the
Hamiltonian but we introduce here an effective Land factor
to incorporate the observed nonantiparallel and the quenching effect in the rare-earth ions in c-sublattice gc gc cos
where is the canting angle that measures the departure
from the collinearity within the c-sublattice and the reducing
of the c-ions magnetic moments see Refs. 19 and 20. It is
worth noticing that, in this work, we associated the reducing
of the c-ion magnetic moment crystal field quenching ef-

M
T

11

dB.
B

In this way S can be calculated from the isothermal magnetization curves. Relation 11 is approximately given by
1
T

ST =

B0

MT + TdB

B0

MTdB ,

12

where T = Ti+1 Ti / 2 and Ti+1 Ti = T is the small temperature variation between the two consecutives isothermal
magnetization curves. Under an adiabatic-isobaric process
the temperature change due to the change in the magnetic
field B : 0 B0 is obtained from the relation

B0

Tad =

T M
CB T

dB,

13

where CB = CBB , T is the total heat capacity at constant

magnetic field and pressure. Usually in magnetic systems the
two main contributions to CB are due to the crystal lattice
Cl = ClT and the magnetic lattice Cm = CmB , T. The first
contribution is usually considered in the Debye approximation and the second ones depend on the magnetic interactions
taken into account in the model magnetic Hamiltonian. The
Cm calculation is not trivial since the Cm should be obtained
from the numerical temperature derivative of the mean thermodynamic magnetic energy UT , B , M = H, which depends on the magnetization. In this way, the Cm calculation
should be included in the self-consistence procedure, for the
magnetization calculation.
Alternatively, from the theoretical point of view, the
magnetic entropy can be directly calculated from the temperature derivative of the free energy. Using Hamiltonian 4,
the free energy is obtained as

F = kT

Nq lnZq,

14

q=a,d,c

where Zq is the partition function of the q-sublattice, given

by

2Jq + 1
xq
2Jq
,
1
sinh
xq
2Jq

sinh
Zq =

15

where xq = BgqJqBq / kT. From free energy 14, the magnetic entropy is obtained as

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053914-3

J. Appl. Phys. 106, 053914 2009

von Ranke et al.

10

Y3Fe5O12

Md /

Ma / ,

M ( / formula unit)

-5

Ma

Md

-10
-15
0

100

200

300

400

500

600

Temperature (K)

FIG. 1. Magnetization vs temperature in Y3Fe5O12. The

open circles represent the experimental data from Ref.
20, and the solid curve represents the theoretical results.
The inset shows the Fe3+ magnetizations in the
a-sublattice and in the d-sublattice.

0
0

100

200

300

400

500

600

700

800

Temperature (K)

ST,B = R

Nqln Zq xqBJ xq,

q=a,d,c
q

16

where R = 8.314 J / mol K is the gas constant. Therefore, the

magnetic entropy change can also be expressed as
S = ST,B = B0 ST,B = 0.

17

It is worth noticing that for high temperature, the Brillouin functions go to zero and the partition functions go to
the total number of quantum magnetic states; i.e., Zq = 2Jq
+ 1. Consequently, the maximum value of the magnetic entropy in R3Fe5O12 / f.u. is given by
Smax = RNa ln2Ja + 1 + Nd ln2Jd + 1
+ Nc ln2Jc + 1.

18

III. MODEL APPLICATION AND DISCUSSIONS

We started determining the three exchange parameters

aa, dd, and ad for Y3Fe5O12. Since Y is a nonmagnetic
ion, this magnetic system is described considering only the
two a- and d-sublattices magnetic state, Eqs. 8 and 9.
Using a numerical self-consistent procedure through the use
of relations 5 and 6 with ac = dc = cc = 0, the sublattices
magnetizations M a and M d can be determined for a given set
of exchange interaction parameters aa, dd, and ad. This set
of parameters was obtained using the experimental magnetization data in the accumulated error , given by

aa, dd, ad =

M exptTi M theorTi
,
M exptTi

19

where M exptTi and M theorTi are the measured

magnetization20,21 and magnetization values theoretically
calculated at temperature Ti, respectively. The accumulated
error is a function of the molecular field parameters variables to be determined by the minimization process. In order to find the best values of the exchange interaction parameters that minimize the error, Powells algorithm22 with
improvements23 was used. In each step of the method used

for minimization, the theoretical magnetization was calculated self-consistently.

The exchange interaction parameters determined by our
best fitting procedure described above were aa
= 101.50 T2 / meV,
ad = 430.88 T2 / meV, and dd
2
= 63.51 T / meV. Our exchange parameters are different
from those obtained by Srivastava et al.20 and show that
more than one set of exchange parameters could be fitted.
Figure 1 shows the temperature dependence of the magnetization M = M a + M d in modulus in Y3Fe5O12 where the open
circles are the experimental data used in relation 19 for the
minimization procedure, and the solid curve represents our
theoretical results. The inset in Fig. 1 displays the a- and
d-sublattices magnetizations versus temperature. The M a
magnetization decreases slower with temperature than the
absolute M d magnetization, since the exchange interaction
between the ions in a-sublattice is greater than the exchange
interaction between the ions in d-sublattice.
Figure 2 shows the temperature dependence of S for
magnetic field changes B : 0 1.6T, obtained using relation
17. The maximum entropy change occurs at Nel temperature at about TN = 565 K and is predicted to be of
0.36 J / mol K for magnetic field changes B : 0 1.6T. Note
that a wide temperature range 200500 K is theoretically
predicted, where the S versus T curve is almost constant
0.09 J / mol K for B : 0 1.6T. This result is directly associated with the M versus T profile showed in Fig. 1, where
the derivative of M is almost constant in the temperature
range 200500 K. From Maxwell relation, the entropy
change can be estimated in this interval S
M / TB 0.09 J / mol K. Materials that exhibit S
as constant as possible in a wide temperature interval of refrigeration are desired in the Ericsson cycle24 since it realizes
that a large temperature spans in the low and high isomagnetic field processes. Theoretical and experimental efforts
have been done in order to understand the mechanisms responsible for the broadening in the MCE peaks desired for
application to magnetic refrigeration.25,26 Unfortunately, we
did not find experimental data for S versus T in Y3Fe5O12

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053914-4

80

Entropy (J/mol.K)

0.4

0.3

-S (J/mol.K)

J. Appl. Phys. 106, 053914 2009

von Ranke et al.

Y3Fe5O12

60
R[3.ln(2Sd+1) + 2.ln(2Sa+1)]
40

B: 0 - 1.6 T

B=0

20

FIG. 2. The temperature dependence of S in

Y3Fe5O12 for a magnetic field change from 0 to 1.6 T.
The inset shows the magnetic entropy vs temperature at
zero magnetic field.

0.2

100

200

300

400

500

600

Temperature (K)

0.1

0.0
0

100

200

300

400

500

600

Temperature (K)

in order to compare with our theoretical prediction. The inset

in Fig. 2 shows the temperature dependence of the total magnetic entropy in Y3Fe5O12 in zero magnetic field. It is worth
noticing that the maximum magnetic entropy is given by
relation 18 neglecting the last term since the Y-ion in
c-sublattice is nonmagnetic.
Figure 3 shows the temperature dependence of Tad for
magnetic field change B : 0 1.6T. The solid curve represents our theoretical results and the points are the experimental data.27 The Debye temperature considered in our model
was D = 392 K. This value was obtained by Parida et al.28
for a similar system Lu3Fe5O12. The peak in the experimental
data of Tad occurs below the theoretical one. This difference can be attributed to the different Y3Fe5O12 samples
used for the measurements of the magnetization Fig. 1 and
Tad Fig. 3. Since we have adjusted the exchange parameters considering the magnetization data, the theoretical Tad
curve peaks at Nel temperature TN = 565 K; see Fig. 1.
The inset shows the magnetic heat capacity versus temperature, for magnetic fields B = 0 and 5 T.

Figure 4 shows the temperature dependence of the magnetization in Dy3Fe5O12 compound. The open circles represent the experimental data19 and the solid curve represents
our theoretical results. The exchange parameters determined
by the above fitting procedure for the Dy3Fe5O12 were
ac = 4.53 T2 / meV,
dc = 26.74 T2 / meV,
and
cc
2
= 2.93 T / meV. The values of other three exchange parameters, aa, ad, and dd, for Dy3Fe5O12 were considered to
present the same values previously determined for Y3Fe5O12.
This consideration is based on the experimental observation
that independently of the type of R ion in the c-sites in
R3Fe5O12, the ferriparamagnetic temperature is relatively
constant, indicating that the Fea Fed interactions are
dominant. The signs in the exchange interactions lead to a
ferromagnetic interaction between Dy and Fea whereas ferrimagnetic interaction between Dy and Fed ions see spins
diagram in Fig. 4. It is expected that the net magnetization,
at T = 0 K, per f.u. in Dy3Fe5O12 to be determined by M 0
= 3gcJc 3gdJd + 2gaJaB = 25B. Nevertheless, due the

100

0.4
Cmag (J/mol K)

80

Tad (K)

0.3

Y3Fe5O12

B=0T
B=5T

60
40
20

Experiment
Theory

0
0

100

0.2

200

300

400

500

600

FIG. 3. The temperature dependence of Tad for

Y3Fe5O12 for a magnetic field change from 0 to 1.6 T.
The open circles represent the experimental data from
Ref. 27, and the solid curve represents the theoretical
results.

Temperature ( K )

0.1

B: 0 - 1.6 T

0.0
0

100

200

300

400

500

600

Temperature (K)
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053914-5

J. Appl. Phys. 106, 053914 2009

von Ranke et al.

20

25

Ma, Md, Mc per

M (Bohr Magnetons / formula unit)

Mc

20

Dy3Fe5O12

18
16
14
12

15

Ma

10
5
0
-5

Md

-10

Tcomp.

-15
0

10

100

200

300

400

500

FIG. 4. The temperature dependence of magnetization

for Dy3Fe5O12. The open circles represent the experimental data from Ref. 19, and the solid curve represents
the theoretical results. The inset shows the three sublattices magnetizations M a, M c, and M d vs temperature.

600

Temperature (K)

c-site d-site a-site

6
4

Dy

3+

Fe

3+

Fe

3+

0
0

100

200

300

400

500

600

Temperature (K)

CEF-quenching effect on the Dy-angular momentum and the

nonantiparallel arrangement between the Dy- and Femagnetic moments as discussed in Sec. II the observed
value M 0 16B in Dy3Fe5O12 yields to = 45.5 in our
model. The inset in Fig. 4 shows the a-, d-, and c-sublattices
magnetizations versus temperature in Dy3Fe5O12 simulated
using Eqs. 810. The magnetization M c decreases faster
with temperature than M a and M d absolute value, since the
exchange interactions between the c-ions are weaker than
those between the a- and a-ions. At the compensation
temperature Tcomp = 217 K, the up magnetic moment in the
a- and c-sublattices equilibrate the down magnetic moment
of the d-sublattice see the vertical dotted line in the inset of
Fig. 4.
Figure 5 shows the temperature dependence of the S
for magnetic field change B : 0 1.6T in Dy3Fe5O12. Three
peaks can be observed in S versus T curve. The higher
and broad one occurs at low temperature T 35 K and is
associated with the large magnetization decreases in low

1.4

160

1.2

Entropy (J/mol.K)

Dy3Fe5O12
B: 0 - 1.6 T

-S (J/mol.K)

1.0
0.8
0.6

temperature see Fig. 4. With increasing temperature, the

second peak appears around Tcomp = 217 K and is negative
S 0, the inverse MCE. The inverse MCE is expected
in ferrimagnetic systems, which exhibit compensation temperature, since the magnetic order increases with increasing
temperature the derivative of M with T, in relation 11, is
positive in the temperature interval where the inverse MCE
is present. Note that between the compensation and Nel
temperatures the magnetization has a maximum at temperature, which we called the inversion-MCE temperature T0. For
Dy3Fe5O12, T0 352 K and as expected from relation 11 it
leads to S = 0; i.e., T0 separates the inverse MCE from the
usual normal MCE S 0. The third peak occurs at TN
570 K and is due to the ferriparamagnetic phase transition. As in Y3Fe5O12, no experimental data are available in
literature for S versus T to compare with our theoretical
results. The inset in Fig. 5 shows the theoretical magnetic
entropy versus temperature for Dy3Fe5O12 without applied

R[3.ln(2Sd+1) + 2.ln(2Sa+1)+3.ln(2Sc+1)]

120

80

B=0

40

0
0

100

200

300

400

500

600

700

Temperature (K)

Tcomp.

0.4

TN

T0

0.2

FIG. 5. The temperature dependence of S in

Dy3Fe5O12 for a magnetic field change from 0 to 1.6 T.
The arrows indicate the compensation temperature
Tcomp, the inversion-MCE temperature T0, and the Nel
temperature TN. The inset shows the entropy vs temperature at zero magnetic field.

0.0
-0.2
0

100

200

300

400

500

600

Temperature (K)
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053914-6

J. Appl. Phys. 106, 053914 2009

von Ranke et al.

100

0.8

Cmag (J/mol K)

Dy3Fe5O12

0.7

Tad (K)

0.6
0.5

60
40
20

Experiment
Theory

0.4

B=0T
B=5T

80

0
0

100

200

300

400

500

600

Temperature ( K )

0.3

B: 0 - 1.6 T

0.2

T0

FIG. 6. The temperature dependence of Tad for

Dy3Fe5O12 for a magnetic field change from 0 to 1.6 T.
The open circles represent the experimental data from
Ref. 27, and the solid curve represents the theoretical
results. The arrow indicates the inversion-MCE temperature T0.

0.1
0.0
-0.1
0

100

200

300

400

500

600

Temperature ( K )

magnetic field. The maximum magnetic entropy occurs

above TN 570 K and is given by relation 18.
Figure 6 shows the temperature dependence of Tad for
magnetic field changes B : 0 1.6T in Dy3Fe5O12. The
open circles represent the experimental data27 and the solid
curve represents our theoretical results. We adopted the Debye temperature D = 327 K in Dy3Fe5O12, which is about
13% less than in Y3Fe5O12. This adopted value is based on
Lindemann law in which, in first approximation, the Debye
temperature is proportional to the inverse of the square root
of the molecular mass of a given compound. The inset shows
the magnetic heat capacity versus temperature, for magnetic
fields B = 0 and 5 T. As in Fig. 5, the inversion-MCE temperature T0 appears at Tad = 0; the sample heats up above T0
and cools down below T0 upon applied magnetic field. No
experimental data are available at low temperature T
10 K to confirm our predicted sharp peak in Tad versus
T.
IV. FINAL COMMENTS

Three coupled magnetic sublattices model in the mean

field approximation has been worked out and used to calculate the MCE in Y3Fe5O12 and Dy3Fe5O12. Our model describes satisfactorily the experimental data for Tad versus T
in both compounds. The rich and complex ferrimagnetic arrangement of Dy3Fe5O12 compound, which exhibits the compensation temperature, was analyzed in terms of the magnetocaloric thermodynamic quantities S and Tad. Unlike in
a simple ferromagnetic system, where only one peak appears
in S and Tad curves, in ferrimagnetic Dy3Fe5O12, three
peaks were predicted. The origins of these peaks were discussed and the occurrence of the compensation temperature
leading to existence of the inverse MCE was explained.
ACKNOWLEDGMENTS

We acknowledge financial support from Conselho Nacional de Desenvolvimento Cientfico e Tecnolgico CNPq,
Brazil and Fundao de Amparo Pesquisa do Estado do Rio
de Janeiro FAPERJ.

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