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Journal of Magnetism and Magnetic Materials 310 (2007) 18661867 www.elsevier.com/locate/jmmm

Magnetic properties, thermal expansion and magnetostriction of Pr0.5Sr0.5CoO3 single crystal

S. Hirahara, Y. Nakai, K. Miyoshi, K. Fujiwara, J. Takeuchi
Department of Material Science, Shimane University, Matsue 690-8504, Japan Available online 30 November 2006

Abstract The measurements of the magnetization, thermal expansion and magnetostriction have been performed on Pr0.5Sr0.5CoO3 single crystals to reveal an unusual anomaly around TA$100 K in a ferromagnetic region below TC$220 K. The magnetization along the [1 1 0] axis in some range of the magnetic eld, e.g. 0.1 T, exhibits a step-like decrease below TA. The isothermal magnetization along the [1 1 0] axis exhibits a step-like increase above HA$1.3 T. A step-like contraction of the lattice length along the [1 1 0] axis is observed for both below TA and above HA. The result indicating a strong correlation between the magnetic state and the lattice suggests that a change of the magnetic easy axis at TA is associated with the d-electron orbital state of Co ions. r 2006 Elsevier B.V. All rights reserved.
PACS: 75.30.m; 75.30.Gw; 75.30.Kz; 75.80.+q Keywords: Cobaltites; Magnetic ordering; Magnetic anisotropy; Magnetostriction; Pr0.5Sr0.5CoO3

Due to the renewed focus on the physics on transition metal oxides, cobalt-based perovskites as well as manganese-based perovskites have been the subject of numerous studies in recent years [1]. A characteristic feature of the perovskite cobalt oxides is that the Hunds rule coupling and the crystal-eld splitting are very close in energy, which results in the different spin states of cobalt ions depending on the crystal structure, temperature, doping concentration and valence state of them. Several studies have recently concentrated on half-doped Ln0.5A0.5CoO3 (Ln rare earth elements, A divalent alkaline elements) oxides because of their complex phase diagram [24]. One of the most interesting materials is Pr0.5Sr0.5CoO3 that shows an unusual step-like behavior of the magnetization at TA$100 K in a ferromagnetic region below TC$220 K [5]. The possibility of a change of the magnetic easy axis associated with the orbital ordering at TA has been pointed out by another work using Lorentz electron microscopy on this material [6]. In order to clarify the anomalous magnetic properties at low temperatures of this material,
Corresponding author. Tel.: +81 852 32 6390; fax: +81 852 32 6409.

E-mail address: jun-tak@riko.shimane-u.ac.jp (J. Takeuchi). 0304-8853/$ - see front matter r 2006 Elsevier B.V. All rights reserved. doi:10.1016/j.jmmm.2006.10.1129

we have performed the magnetization, thermal expansion and magnetostriction measurements on Pr0.5Sr0.5CoO3 single crystals. Single crystals of Pr0.5Sr0.5CoO3 were successfully grown by the oating-zone furnace method with four pairs of ellipsoidal mirror and halogen lumps under a controlled atmosphere. The crystal structure was found by X-ray diffraction to be monoclinic (P21/m) in accordance with earlier reports [5,6]. We used the tetragonal notation for simplicity, based on the cell 21/2a 21/2a 2a (a being the cubic perovskite lattice parameter). The magnetization was measured using a SQUID magnetometer. The thermal expansion and magnetostriction under magnetic elds up to 7 T were measured with a strain gauge method. Fig. 1 shows the temperature dependence of the magnetization M measured in 0.1 T magnetic eld under eld-cooled (FC) conditions (upper panel). The magnetization along the [1 0 0] axis exhibits a step-like increase below TA. In contrast, the magnetization along the [1 1 0] axis exhibits a step-like decrease below TA. The magnetization along the [0 0 1] axis exhibits a small step-like increase below TA and has a smaller value than those for the other two axes at all temperatures. Note that the magnetization

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S. Hirahara et al. / Journal of Magnetism and Magnetic Materials 310 (2007) 18661867 1867

30 [100] [110] M [emu/g] 20 [001] Pr0.5Sr0.5CoO3 H=0.1T

2
Pr0.5Sr0.5CoO3

[100] [110] [001]

T=10K

M [ B/f.u.]

1
B/f.u.]

2 3 1 1 [ 110]

M[ 0 0

10

0 100 0.002 L/L H=0 T 200 [110]

0 1 0

[110]

T=150K

L/L

-0.002

-0.002

T=70K

H=7 T
T=10K

100 T [K]

200

300

-0.004 0 1 2 H [T]
Fig. 2. Magnetization (upper panel) and magnetostriction (lower panel) for Pr0.5Sr0.5CoO3 as a function of applied eld.

Fig. 1. Temperature dependence of the magnetization (upper panel) and the thermal expansion (lower panel) for Pr0.5Sr0.5CoO3.

measured in such a small eld as 0.01 T exhibits a step-like decrease below TA for all three axes. And also note that these step-like behaviors are only observed for 0.4pxp0.55 in Pr1xSrxCoO3. Lower panel of Fig. 1 shows the temperature dependence of the linear thermal expansion, where DLXL means relative length change normalized at T 10 K and H 0. A step-like contraction of the lattice length along the [1 1 0] axis below TA can be seen in the gure, which is largely enhanced in a 7 T eld. Fig. 2 shows the isothermal magnetization at 10 K as a function of an applied magnetic eld (upper panel). The magnetization along the [1 0 0] axis exhibits a sharp increase and approaches to the saturated value as the eld is increased. In contrast, the magnetization along the [1 1 0] axis exhibits a step-like increase above HA$1.3 T. This increased magnetization is kept when the eld is reduced below HA, which leads to a large hysteresis as shown in an inset of the gure. Lower panel of Fig. 2 shows the magnetostriction along the [1 1 0] axis as a function of an applied magnetic eld being parallel to the [1 1 0] axis at 10, 70 and 150 K. A steplike contraction of the lattice length above HA can be seen at the temperature below TA as an applied eld is increased. This contracted length is kept even after an applied eld is reduced to zero again.

These results imply that the easy axis changes from [1 1 0] to [1 0 0] through TA as the temperature is reduced. The energy difference between the two states with a different easy axis is small because higher-temperature state with an [1 1 0] easy axis induced by an applied eld at low temperatures is kept even after the eld is reduced to zero as a metastable state. The behaviors of the thermal expansion and magnetostriction indicate a strong correlation between the magnetic state and the lattice. This suggests that a change of the magnetic easy axis at TA is associated with the d-electron orbital state of Co ions.

References
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