See discussions, stats, and author profiles for this publication at: https://www.researchgate.

net/publication/234506421

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

CITATIONS READS

6 443

3 authors:

Zhaosen Liu Martin Diviš

Hengyang Normal University Charles University in Prague
62 PUBLICATIONS   343 CITATIONS    260 PUBLICATIONS   2,718 CITATIONS   

SEE PROFILE SEE PROFILE

Vladiimir Sechovsky
Charles University in Prague
735 PUBLICATIONS   7,726 CITATIONS   

SEE PROFILE

Some of the authors of this publication are also working on these related projects:

Physics of UIrSi3 View project

PhD Thesis : Characterization of crystal-field and phonon coupling in RE1+xBa2-xCu3O6+y antiferromagnets View project

All content following this page was uploaded by Zhaosen Liu on 25 November 2014.

The user has requested enhancement of the downloaded file.

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

°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 = with the experimental data.[28] The theoretical curves
2.89 meV, A44 = −84.4 meV, A06 = −1.92 meV and in the two directions show reasonable agreement with
A46 = 22.6 meV, respectively, by Gasser et al. with an the measured data. In particular, the theoretical curve
extrapolation approach.[24] Using the CFPs and J ’s along the easy a-axis starts to grow from almost zero
given above, we firstly calculate the spontaneous mag- at very low temperatures, increases gradually with the
netizations for the two sorts of Tb ions at low temper- rising temperature, exhibits a sharp peak at TN , then
atures as displayed in Fig. 1. The crystalline exhibits decays afterwards as observed in the experiment.
strong magnetic anisotropy below TN , its magnetic
moments only orders spontaneously in the ab-plane. 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.
the two sublattices are usually of relatively very large
Expt. 6 K
magnitude well below TN . However they mutually
50 Calc. 6 K
offset, so that their sum values, which are usually ob-
served in experiments, show much weaker but reason-
J1=0.530 K, J2=-0.335 K
able magnitude. As a result, the overall susceptibility
0 in the easy direction increases gradually from almost
0 10 20 30 40 50 60 zero at very low temperatures to a maximum at TN
(kOe)
as shown in Fig. 2 and 3. These typical characters of
Fig. 5. Calculated magnetization curves of TbNi2 B2 C at the antiferromagnets are well described by our two-
T = 6, 12 and 20 K versus the external field applied in the sublattice model. Of course, to study the magnetic
a-direction in comparison with experimental results.[22]
The curves for T = 12 and 20 K are shifted along the ver-
process of rare-earth antiferromagnets with more com-
tical axis for clarity with 50 and 100 units, respectively, as plicated magnetic structures, a many-sublattice model
carried out by the previous authors.[22] Here J1 = 0.530 K is required, however more RKKY exchange constants
and J2 = -0.335 K are used. are then involved and needed to be determined. Con-
sequently, the computations become tedious or simply
To further test our two-sublattice model and impossible. However, with this two-sublattice model,
demonstrate its utility, we also calculate the magneti- we are able to evaluate the susceptibility and magnetic
zation curves of the compound at a few fixed temper- moment of each sort of magnetic ion or sublattice sep-
atures T = 20, 60, and 200 K in an external magnetic arately, to simulate the magnetic process and study
field varied up to 120 kOe along the easy a-axis. The the magnetic properties of rare-earth antiferromagnets
theoretical results are displayed in Fig. 4 in compar- in low temperature region at least qualitatively.
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 References
the experimental ones. The deviation at T = 20 K [1] Maple M B 1995 Physica B 215 110
in the field higher than 70 kOe might be attributed to [2] Cho B K, Canfield P C and Johnston D C 1995 Phys. Rev.
the quadrupole interaction and magneto-elastic effects B 52 3844

067501-3
 CHIN. PHYS. LETT. Vol. 26, No. 6 (2009) 067501

[3] Huang Q, Sontoro A, Grigereit T E, Lynn J W, Cava R J, [15] Siegrist T, Zandbergen H W, Cava R J, Krajewski J J and
Krajewski J J and Peck Jr W F 1995 Phys. Rev. B 51 3701 Peck J W F 1994 Nature 367 254
[4] Sinha S K, Lynn J W, Grigereit T E, Hossain Z, Gupta L [16] Huang Q, Lynn J W, Santoro A, Chakoumakos B C, Cava
C, Nagarajan R and Godart C 1995 Phys. Rev. B 51 681 R J, Krajewski J J and Peck J W F 1996 Physica C 271
[5] Zarestky J, Stassis C, Goldman A I, Canfield P C, Derve- 311
nagas P, Cho B K and Johnston D C 1995 Phys. Rev. B [17] Chang L J, Tomy C V, Paul D M, Andersen N H and Yethi-
51 678 raj M 1996 J. Phys.: Condens. Matter 8 2119
[6] Moshe Kuznietz and Hiroyuki Takeya 2000 Physica B 281 [18] Skanthakumar S and Lynn J W 1999 Physica B 259–261
& 282 1004 576
[7] Lee W C 2007 Physica 399 116 [19] Bitterlich H, Loser W, Behr G, Nenkov K, Fuchs G, Belger
A and Schultz L 1998 Physica C 308 243
[8] Grigereit T E, Lynn J W, Huang Q, Santoro A, Cava R J,
[20] Dervenagas P, Zarestky J, Stassis C, Goldman A I, Canfield
Krajewski J J and Peck J W F 1994 Phys. Rev. Lett. 73
P C and Cho B K 1996 Phys. Rev. B 53 8506
2756
[21] Kreyssig A, Stockert O, Reznik D, Woodward F M, Lynn
[9] Goldman A I, Stassis C, Canfield P C, Zarestky J, Dervena-
J W, Bitterlich H, Souptel D, Behr G and Loewenhaupt M
gas P, Cho B K, Johnston D C and Sternlieb B 1994 Phys.
2004 Physica C 408–410 100
Rev. B 50 9668
[22] Tomy C V, Afalfiz L A, Lees M R, Martin J M and Paul D
[10] Chang L J, Tomy C V, Paul D M and Ritter C 1996 Phys. McK 1996 Phys. Rev. B 53 307
Rev. B 54 9031 [23] Gasser U, Allenspach P, Fauth F, Henggeler W, Mesot J
[11] Lynn J W, Skanthakumar S, Huang Q, Sinha S K, Hossain and Furrer A 1996 Z. Phys. B 101 345
Z, Gupta L C, Nagarajan R and Godart C 1997 Phys. Rev. [24] Gasser U, Allenspach P, Mesot J and Furrer A 1997 Physica
B 55 6584 C 282-287 1327
[12] Kreyssig A, Lowenhaupt M, Muller K H, Fuchs H G, Hand- [25] Liu Z S, Diviš M and Sechovský V 2008 Phys. Rev. B 78
stein A and Ritter C 1997 Physica B 234 737 214409
[13] Eisaki H, Takagi H, Cava R J, Mizuhashi K, Lee J O, Bat- [26] Liu Z S, Diviš M and Sechovský V 2009 Phys. Status Solidi
logg B, Krajewski J J, Peck J W F and Uchida S 1994 Phys. B 246 448
Rev. B 50 647 [27] Liu Z S, Diviš M and Sechovský V 2009 Phys. Status Solidi
[14] Ribeiro R A, Bud’ko S L and Canfield P C 2003 J. Magn. B DOI: 10.1002/pssb.200844491
Magn. Mater. 267 216 [28] Cho B K 1998 Physica C 298 305

067501-4

View publication stats