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CONDENSED MATTER: ELECTRONIC STRUCTURE, ELECTRICAL, MAGNETIC,

AND OPTICAL PROPERTIES: The Magnetic Properties of TbNi2B2C
Investigated with a Two-Sublattice Model

Article  in  Chinese Physics Letters · May 2009

DOI: 10.1088/0256-307X/26/6/067501

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 CHIN. PHYS. LETT. Vol. 26, No. 6 (2009) 067501

∗
Magnetic Properties of TbNi2 B2 C Investigated with a Two-Sublattice Model
LIU Zhao-Sen(4ìÜ)1∗∗ , Diviš Martin2 , Sechovský Vladimir2
1
Faculty of Mathematics and Physics, Nanjing University of Information Science and Technology, Nanjing 210044
2
Department of Condensed Matter Physics, Faculty of Mathematics and Physics, Charles University, Ke Karlovu 5,
121 16 Prague 2, Czech Republic

(Received 2 February 2009)

A two-sublattice model for rare-earth antiferromagnets is employed to study the magnetic properties of TbNi2 B2 C.
The theoretical susceptibility and magnetization curves obtained with the model show reasonable agreements with
the experimental results.

PACS: 75. 10. Dg, 75. 10. −b, 75. 50. Ee

The rare-earth nickel borocarbides RNi2 B2 C have
attracted considerable research interest for many
years because of the coexistence of superconductiv-
ity and long-range magnetic ordering observed in
these materials.[1−14] All members of this isostruc-
tural family crystallize in the tetragonal ThCr2 Si2
structure.[15−17] X-ray diffraction experiment revealed
that the R-C layers alternate with the Ni2 B2 layers
along the c-axis, and the lattice constants a and c,
as well as the z position of boron, scale roughly with
the ionic radius of the rare earth. Neutron diffrac-
tion experiments found that the magnetic ordering
in this system arises solely from the rare earth ions
which bear localized 4f electrons, no ordered mag-
netic moment was detected on the Ni site.[18] In con-
trast to other members, TbNi2 B2 C shows no super-
conductivity at least down to 7 mK.[18] It orders in
an incommensurate antiferromagnetic structure below
TN = 15 K with the magnetic Tb moments aligned
along the a-axis.[19−22]
In order to study the magnetic and thermody-
namic properties of the RNi2 B2 C compounds quan-
titatively, Gasser et al. performed inelastic neutron
scattering experiment to determine the crystal-field
parameters (CFPs) for the compounds with R = Ho,
Er and Tm.[23,24] They then calculated the suscepti-
bilities and magnetic specific heats of these materials
by using the CFPs they had got, and obtained good
agreements with experimental data above the mag-
netic transition temperatures.[23] However below TN ,
their theoretical susceptibility curves along the easy
axes all tend to very large values, exhibiting evident
deviation from the experimental results.
Obviously, to reproduce the magnetic ordering of
a rare-earth antiferromagnet below its Néel temper-
ature theoretically, RKKY exchange interaction be-
tween the neighboring magnetic ions must be consid-
ered. In addition, at temperatures well below TN , the
material remains antiferromagnetic even being placed
in a weak external magnetic field. Therefore, to de-
scribe the magnetic structure of an antiferromagnet
in a magnetic phase, the single-sublattice model used
by previous authors is obviously inadequate, a new
model which mimics the magnetization process of the
two sublattices with opposite magnetic moments be-
low TN has to be built and utilized. For this purpose,
we have proposed a modified two-sublattice model and
successfully used it to study the magnetic properties of
HoNi2 B2 C and DyFe2 Si2 .[25−27] In the present work,
we have employed the model once again to investigate
the magnetic behaviors of TbNi2 B2 C as described in
detail in the following.
In this model, the rare-earth A and B ions which
form two sublattices are all under the interaction of
the crystal-electric field (CEF) produced by the sur-
rounding electric charges; the A ion interacts with an-
other A ion and a B ion nearby through RKKY ex-
change interaction with coupling constants J11 and
J12 , the B ion with another B ion and the A ion
nearby with coupling constants J22 and J21 , respec-
tively. Hence, the Hamiltonian of the system with the
two sublattices can be expressed with
H(A) = HCF − J11 J · hJ (A) i − J12 J · hJ (B) i
− µB gJ B · J ,
H (B)
= HCF − J22 J · hJ (B) i − J21 J · hJ (A) i
− µB gJ B · J , (1)
where HCF stands for CEF interaction, and reads
HCF = A02 Y20 + A04 Y40 + A44 Y44 + A06 Y60 + A46 Y64 , (2)
for the RNi2 B2 C series of the tetragonal crystal
structure.[23,24]
To simplify the model and facilitate the computa-
tions, we set J11 = J22 = J1 and J12 = J21 = J2 ,
which were found to be J1 = 0.530 K and J2 =
−0.335 K for TbNi2 B2 C by fitting its measured sus-
ceptibility curves and TN .[28]

∗ Supported by the Natural Science Foundation of Jiangsu Province under Grant No BK2008438, and the Ministry of Education

of the Czech Republic under Grant No MSM 0021620834.

∗∗ Email: liuzhs@yahoo.com.cn

°c 2009 Chinese Physical Society and IOP Publishing Ltd

067501-1
 CHIN. PHYS. LETT. Vol. 26, No. 6 (2009) 067501

The crystal-field parameters (CFPs) of TbNi2 B2 C as functions of temperature in Fig. 2 in comparison

have been found to be A02 = −15.4 meV, A04 =
2.89 meV, A44 = −84.4 meV, A06 = −1.92 meV and
A46 = 22.6 meV, respectively, by Gasser et al. with an
extrapolation approach.[24] Using the CFPs and J ’s
given above, we firstly calculate the spontaneous mag-
netizations for the two sorts of Tb ions at low temper-
atures as displayed in Fig. 1. The crystalline exhibits
strong magnetic anisotropy below TN , its magnetic
moments only orders spontaneously in the ab-plane.
with the experimental data.[28] The theoretical curves
in the two directions show reasonable agreement with
the measured data. In particular, the theoretical curve
along the easy a-axis starts to grow from almost zero
at very low temperatures, increases gradually with the
rising temperature, exhibits a sharp peak at TN , then
decays afterwards as observed in the experiment.
4

10-3 cm3/g)
Our calculations always generate positive moments for J1=0.530 K, J2=-0.335 K

the A ion, but negative ones for the B ion below TN , 1000 3 =0.01 T
Calc.
manifesting the antiferromagnetic nature of the rare- 2 //

10-3 cm3/g)

(
earth magnet.
500 1

/
9 0
0 20 40 60 80 100 120 140
J1=0.530 K, J2=-0.335 K
0 (K)

(
6

/
A Subllatice

3 -500
B Sublattice

J1=0.530 K, J2=-0.335 K
=0.01 T
(mB/Tb)

// ,

0
0 10 20 30 40 50
A ion (K)
-3
M

B ion
Fig. 3. Calculated susceptibility of A and B sublat-
-6 tices, respectively, as well as their sum values (inset) of
TbNi2 B2 C versus temperature with the external mag-
netic field applied in the a-direction for J1 = 0.530 K and
-9 J2 = −0.335 K.
0 5 10 15 20 25
(K) To understand the magnetic process involved at
low temperatures, we display in Fig. 3 the susceptibil-
Fig. 1. Calculated magnetization curves of the A and
B ions of TbNi2 B2 C versus temperature in the absence ity curves of the two sublattices and their sum values,
of external magnetic field, with the exchange constants which are actually measured in the experiment, along
J1 = 0.530 K and J2 = −0.335 K. the a-direction as functions of temperature. As shown
in the figure, the magnetic moment of the A ion al-
ways aligns along the a-axis, the susceptibility of the A
4 Expt. //
sublattice decays gradually from 782.77 × 10−3 cm3 /g
Calc. //

Expt. //
at T = 0.1 K, an extremely larger value than that
10-3 cm3/g)

3 Calc. //
measured at the temperature, to 2.28 × 10−3 cm3 /g
when the temperature is rising to TN = 15 K. On the
J1=0.530 K, J2=- 0.335 K, =0.01 T other hand, the B moment orders in the negative a-
2 axis below TN , that is, antiparallel to the external
field; the susceptibility of the B sublattice starts from
(

−782.66 × 10−3 cm3 /g at T = 0.1 K, which slightly

1 differs from that of the A sublattice at the same tem-
perature, then attenuates continuously due to the dis-
0 turbance of increasing temperature, and jumps sud-
0 30 60 90 120 150 denly from a negative value −63.14 × 10−3 cm3 /g at
(K) T = 14.9 K to 1.76 × 10−3 cm3 /g at TN = 15 K, then
Fig. 2. Calculated susceptibilities of TbNi2 B2 C versus
decreases slowly afterwards. The relatively very large
temperature with external magnetic fields applied in the opposite moments of the two sublattices offset. As a
a- and c-directions, respectively, in comparison with the result, the overall susceptibility of the antiferromag-
experimental results,[28] for J1 = 0.530 K and J2 = net exhibits much weaker but reasonable magnitude
−0.335 K.
below TN , it increases gradually from zero with the ris-
With the above parameters, we then calculate the ing temperature, reaches a maximum at TN , and then
susceptibility data with the external magnetic fields abates afterwards as shown in Fig. 2 and in the inset of
of 0.01 T assumed to be exerted along the a and c Fig. 3. However, when the external magnetic field of
axes, respectively, such obtained results are depicted the same strength is exerted in the hard c-direction,

067501-2
 CHIN. PHYS. LETT. Vol. 26, No. 6 (2009) 067501

the theoretical susceptibilities of the two sublattices which are usually induced by a strong external mag-
are found to be almost identical in the whole temper- netic field in the compounds containing heavy rare-
ature range, thus the overall susceptibility is simply earth elements.
equal to 2 times of each sublattice. Figure 5 displays the magnetization curves of
TbNi2 B2 C calculated at a few low temperatures, pro-
160 vided again that the external field is exerted in the
J1 = 0.530 K, J2 = - 0.335 K
a-direction. For comparison the experimental results
Calc. 20 K are also depicted here[22] . As carried out by the previ-
120 Expt. 20 K
ous authors, the curves for T = 12 and 20 K are shifted
up along the vertical axis by 50 and 100 units respec-
(emu/g)

Calc. 60 K tively for clarity. The curve for T = 20 K has already

80 60 K
Expt. been plotted in Fig. 4. Now our new curve obtained
at T = 12 K shows excellent agreement with the ex-
200 K
perimental data, and the one calculated at T = 6 K
40 Calc.
Expt. 200 K exhibits similar tendency and magnitude to the exper-
imental curve, especially a field-induced phase transi-
0 tion around H = 22 kOe is reproduced, meaning that
0 20 40 60 80 100 120 our model is able to describe the magnetic properties
(kOe) below TN reasonably.
In conclusions, we have studied the magnetic prop-
Fig. 4. Calculated magnetization curves of TbNi2 B2 C at
T = 20, 60 and 200 K versus the external field applied erties of TbNi2 B2 C with the two-sublattice model,
in the a-direction in comparison with the experimental and obtained good agreement with the experimental
results,[22] for J1 = 0.530 K and J2 = −0.335 K. results. Obviously, the magnetization and suscepti-
bility of a rare-earth antiferromagnet measured below
Expt. 20 K TN actually represent the overall values of the two
200 Calc. 20 K antiferromagnetically coupled magnetic ions or sub-
lattices. Even in a weak external magnetic field, the
two sorts of magnetic moments still align in the op-
150
(emu/g)

posite directions well below the Néel temperature. As

found in our calculations, the susceptibility values of
12 K
100 Calc.

12 K
Expt.
Expt. 6 K
50 Calc. 6 K
J1=0.530 K, J2=-0.335 K
0 in the easy direction increases gradually from almost
0 10 20 30 40
(kOe)
Fig. 5. Calculated magnetization curves of TbNi2 B2 C at
T = 6, 12 and 20 K versus the external field applied in the
a-direction in comparison with experimental results.[22]
The curves for T = 12 and 20 K are shifted along the ver-
tical axis for clarity with 50 and 100 units, respectively, as
carried out by the previous authors.[22] Here J1 = 0.530 K
and J2 = -0.335 K are used.
To further test our two-sublattice model and
demonstrate its utility, we also calculate the magneti-
zation curves of the compound at a few fixed temper-
atures T = 20, 60, and 200 K in an external magnetic
field varied up to 120 kOe along the easy a-axis. The
theoretical results are displayed in Fig. 4 in compar-
ison with the experimental data measured by Tomy
et al.[22] Our theoretical curves at these temperatures
exhibit the tendency and magnitude very similar to
the experimental ones. The deviation at T = 20 K
in the field higher than 70 kOe might be attributed to
the quadrupole interaction and magneto-elastic effects
the two sublattices are usually of relatively very large
magnitude well below TN . However they mutually
offset, so that their sum values, which are usually ob-
served in experiments, show much weaker but reason-
able magnitude. As a result, the overall susceptibility
50 60 zero at very low temperatures to a maximum at TN
as shown in Fig. 2 and 3. These typical characters of
the antiferromagnets are well described by our two-
sublattice model. Of course, to study the magnetic
process of rare-earth antiferromagnets with more com-
plicated magnetic structures, a many-sublattice model
is required, however more RKKY exchange constants
are then involved and needed to be determined. Con-
sequently, the computations become tedious or simply
impossible. However, with this two-sublattice model,
we are able to evaluate the susceptibility and magnetic
moment of each sort of magnetic ion or sublattice sep-
arately, to simulate the magnetic process and study
the magnetic properties of rare-earth antiferromagnets
in low temperature region at least qualitatively.
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