Proceedings of the International Conference on Strongly Correlated Electron Systems (SCES2013)

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Proc. Int. Conf. Strongly Correlated Electron Systems (SCES2013)
JPS Conf. Proc. 3, 015044 (2014)
http://dx.doi.org/10.7566/JPSCP.3.015044

Pressure-Induced Magnetic Transition and Disappearance

of Superconductivity in CeNiGe3
∗
Yoichi Ikeda1, , Takeshi Tomijima1 , Shingo Araki1 , Tatsuo C. Kobayashi1 and Keizo
Murata2
1
Graduate School of Natural Science and Technology, Okayama University, 3-1-1 Tsushima-naka,
Okayama 700-8530, Japan
2
Division of Molecular Materials Science, Graduate School of Science, Osaka City University,
Osaka 558-8585, Japan
E-mail: kobayashi@science.okayama-u.ac.jp
(Received October 18, 2013)

Pressure-temperature phase diagram of CeNiGe3 is reinvestigated with electrical resistivity measure-

ment up to p ∼ 4 GPa utilizing a single crystal under the better hydrostatic condition. We discovered
that the new successive phase transition appears above p ∼ 3.7 GPa in the antiferromagnetic phase
(AFM-I), and the superconductivity disappears simultaneously. The application of magnetic field
along the a-axis suppresses the successive transition, indicating that the new pressure-induced phase
is considered as an antiferromagnetic phase (AFM-II) with a small magnetization compared with
that of the AFM-I phase. We found that the ordered state in the AFM-II phase is conclusively dif-
ferent from the commensurate AFM-I state which was observed in the previous nuclear-quadrupole-
resonance study, and the superconductivity can coexist with the commensurate AFM-I state, but not
with the AFM-II state.
KEYWORDS: superconductivity, antiferromagnetism, pressure effect, CeNiGe3 . . .

1. Introduction

Unconventional superconductivity in Ce-based compounds has been a hot topic in the scope of
the heavy fermion physics including magnetism and quantum critical phenomena. In CePd2 Si2 [1],
CeIn3 [1], and CeRh2 Si2 [2], pressure-induced superconductivity was observed in the vicinity of the
antiferromagnetic (AFM) quantum critical point at which the Néel temperature goes down to zero
(T N = 0 K). Among these compounds, it is plausible that spin fluctuations mediate the superconduc-
tivity. On the other hand, CeCu2 Si2 [3] and CeXIn5 (X = Co, Rh, Ir) [4–6] exhibit superconductivity
in a wide pressure range that is extended toward the paramagnetic (PM) region. For CeCu2 Si2 and
CeCu2 Ge2 , the superconducting (SC) transition temperature T sc shows a marked increase far from
a magnetic critical pressure pc , and subsequently disappears at higher pressures [3, 7]. The valence
crossover scenario was proposed theoretically by K. Miyake and his co-workers to interpret the en-
hancement of T sc in these materials, where the plausible critical valence fluctuations possibly give
rise to the enhancement of T sc [8].
An antiferromagnet CeNiGe3 has an orthorhombic SmNiGe3 -type structure (Cmmm; space group
No. 65) with inversion symmetry, and also shows pressure-induced superconductivity in a wide pres-
sure range [9, 10]. The pressure-temperature (p-T ) phase diagram was investigated with electrical
resistivity measurements by using polycrystalline sample as shown in Fig. 1. The Néel temperature

∗
Present address: Neutron Science Laboratory, The Institute for Solid State Physics, The University of Tokyo, 5-1-5
Kashiwanoha, Kashiwa, Chiba 277-8581, Japan

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015044-1 ©2014 The Physical Society of Japan
 Proceedings of the International Conference on Strongly Correlated Electron Systems (SCES2013)
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JPS Conf. Proc. 3, 015044 (2014) 015044-2

10
TN Kotegawa
8
Harada
6 AFM Tx
T (K)

I
AFM
4 II
Tsc×5
TA
2

0
0 2 4 6 8 10
p (GPa)
Fig. 1. Pressure-temperature phase diagram of CeNiGe3 . T N (kink in ρ(T )), T x (peak in dρ(T )/dT ) and T sc
(ρ = 0) are depicted by closed circles (blue), diamonds (red), and triangles (green), respectively. The values
of T sc are scaled by a factor of five in this figure. Open circles and small dots indicate T N and T sc , which are
determined by H. Kotegawa et al. with resistivity measurements by using polycrystalline samples [10]. Open
squared symbols denote T A determined by A. Harada et al. with NQR measurement [12].

T N , which is denoted by open circles, initially increases with increasing pressure up to 3 GPa, and
subsequently decreases at higher pressures. The critical pressure for T N was estimated to be about
pc ∼ 7 GPa [10]. Interestingly, partially overlapped two SC domes were observed in CeNiGe3 , as
seen in Fig. 1, where T sc is indicated by small dots. A first SC dome emerges from ∼ 1.7 GPa, and is
embedded in the deep inside of the AFM phase. This SC state becomes fragile at higher pressures, and
may disappear in the intermediate pressure range of 4.0-5.4 GPa, where the zero resistance was not
observed. Subsequently, superconductivity revives in a further high-pressure region, and T sc shows a
maximum around the AFM critical point pc ∼ 7 GPa.
The residual resistivity ρ0 strikingly increases with increasing pressure: ρ0 at pc is about ∼ 100-
times as large as that at ambient pressure. This striking increase is extrinsic and is possibly caused
by an increase in micro-crack and/or residual strain in the polycrystalline sample. We speculated that
the large anisotropy of the compressibility in CeNiGe3 [11] may cause the micro cracks along of the
grain boundary. Therefore, the increase in ρ0 leads to a decrease in mean free path of conduction
electrons, and may influence the emergence and the broadening of the two SC phases in CeNiGe3 .
A 73 Ge-nuclear quadrupole resonance (NQR) measurement was carried out with 73 Ge-enriched
polycrystalline samples under high pressure up to 2.8 GPa [12]. The temperature variation of the
NQR spectrum revealed that a crossover from an incommensurate AFM state to a commensurate
AFM state occurs at T A (< T N ) under high pressure, depicted by open squared symbols in Fig. 1.
The existence of the incommensurate AFM state has also been pointed out in the preceding report
of the neutron diffraction experiment with powder samples at ambient pressure [13]. The nuclear
spin-lattice relaxation rate 1/T 1 disclosed that the unconventional superconductivity emerges in the
commensurate AFM state. In addition, an enhancement of the nuclear spin-spin relaxation rate 1/T 2
takes place at T A , indicating the development of low-lying magnetic excitations even in the deep
inside of the AFM phase. They suggested that the longitudinal spin-density fluctuations may be a
possible glue of the superconductivity in the AFM phase of CeNiGe3 .
Our motivation in the present study is to investigate the unusual SC domes in CeNiGe3 in further
detail, in order to reconfirm the unusual p-T phase diagram with electrical resistivity measurement by

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 Proceedings of the International Conference on Strongly Correlated Electron Systems (SCES2013)
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JPS Conf. Proc. 3, 015044 (2014) 015044-3

12
3.9 GPa 3.9
150 3.7 3.7
3.5
3.0
2.3 8
ρ (µΩ cm)

ρ (µΩ cm)
100 1.6 3.5
ambient

3.0
2.3 4
50
I || c 1.6
ambient
CeNiGe3 (a) (b)
0 300 0
1 10 100 0 0.1 0.2 0.3 0.4 0.5
T (K) T (K)
Fig. 2. (a) The electrical resistivity of CeNiGe3 as a function of temperature (logarithmic T -scale) at several
pressures. (b) Low-temperature part of the resistivity.

using single crystalline sample under the better hydrostatic condition, and to clarify the coexistence
state of superconductivity with antiferromagnetism in CeNiGe3 . The magnetic-field effect is also
investigated.

2. Experimental

A single crystal of CeNiGe3 is prepared by the Ni-Ge self-flux method as described in ref. 14. For
our sample, the residual resistivity ratio (RRR) at ambient pressure is estimated to be about 50, which
is the same value as that of the polycrystal in the previous study [12]. Pressure is applied by using
an indenter-type pressure cell up to ∼ 4 GPa [15] with Daphne oil 7474 as the pressure-transmitting
medium. The solidification pressure of Daphne 7474 is about ∼ 3.7 GPa at room temperature (∼ 300
K) and ∼ 6.7 GPa at 100◦ C [16]. Therefore, pressure was applied to a sample at ∼ 60◦ C in order
to improve the hydrostaticity. The pressure value is determined from T sc of lead [17]. Electrical
resistivity is measured down to 60 mK using a dilution refrigerator with a conventional four terminal
method utilizing an auto AC resistance bridge (LR700; Linear Research Inc.), and the electric current
is applied along the c-axis.

3. Results and Discussion

Figures 2 (a, b) shows the temperature dependence of the electrical resistivity of CeNiGe3 at
several pressures. The superconductivity is not observed at ambient pressure down to 60 mK even
for the single crystal (Fig. 2 (b)). At ambient pressure, the resistivity shows a concave-downward
anomaly around 100 K and a plateau around 10 K. Thinking of the excited crystalline-electric-field
(CEF) levels of CeNiGe3 which lie around 100 and 170 K [14, 18], the bump anomaly around 100 K
can be interpreted as a decrease in spin-disorder scatterings associated with the excited CEF states,
and the plateau around 10 K is mainly derived from the paramagnetic scatterings from the magnetic
moment of the ground state in a qualitative picture. The magnetic scatterings suddenly decrease below
T N ∼ 5.3 K, and subsequently ρ(T ) shows a temperature-independent residual resistivity (ρ0 ∼ 2.3

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 Proceedings of the International Conference on Strongly Correlated Electron Systems (SCES2013)
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JPS Conf. Proc. 3, 015044 (2014) 015044-4

200
(a) CeNiGe3 TN +60 (b)
3.9 GPa
3.7 +40
150 Tx

dρ / dT (arb. unit)
3.5 3.9
+25
ρ (µΩ cm)

3.0
2.3 +20 3.7
100 1.6
ambient 3.5
+15

+10 3.0
50 2.3

+0 1.6
I || c
0
0 2 4 6 8 10 0 2 4 6 8 10
T (K) T (K)
Fig. 3. (a) Temperature dependence of the electrical resistivity of CeNiGe3 around the Néel temperature,
where the origin of each curves is moved in the vertical direction for clarity. (b) Temperature dependence of
dρ/dT at several pressures.

µΩ cm at ambient pressure) as shown in Fig. 2 (b). The Kondo effect seems to be weak at ambient
pressure: the fact that the Kondo temperature of CeNiGe3 which is estimated to be T K ∼ 4.5 K at
ambient pressure from specific heat [18] is smaller than T N . On the other hand, at high pressures, the
resistivity exhibits the characteristic “− ln T ”-like upturn in a high-temperature regime, implying the
enhancement of the Kondo effect due to an increase in the cf hybridization with increasing pressure.
As seen in Fig. 2 (b), a clear zero-resistance associated with the pressure-induced superconduc-
tivity is observed above p ∼ 2.3 GPa, and suddenly disappears above p ∼ 3.7 GPa for the single
crystal. Pressure dependence of T sc is plotted in Fig. 1 with (green) reversed triangles. The present
results are qualitatively consistent with the previous results which are denoted by small dots in Fig.
1 [10]. In addition, the pressure dependence of the residual resistivity is also consistent with the pre-
vious results within the present pressure range (p . 4 GPa). However, the emergent pressure of the
superconductivity for the single crystal is higher than that for the polycrystals, and the T sc of the
single crystal is smaller than that of the previous results in an entire pressure range [10].
As mentioned above, the resistivity exhibits a kink anomaly at T N which is denoted by (blue) ar-
rows in Fig. 3 (a). Pressure dependence of T N is summarized in Fig. 1 with closed (blue) circles, and
fully reproduces the previous results for the polycrystals [10]. However, in contrast to the 73 Ge-NQR
measurement [12], the pressure-induced magnetic crossover at T A from the incommensurate AFM to
the commensurate AFM state is not observed in the present resistivity measurement: the correspond-
ing anomaly at T A is not detected in the ρ(T ) and the temperature differential of the resistivity dρ/dT
as seen in Figs. 3 (a) and (b). Note that the crossover has not been identified in previous macroscopic
measurements [10] even in the calorimetric study under high pressure [19]. We speculate that a “grad-
ual change” of the magnetic property, for example, temperature variation of the ordering vector, may
obscure the corresponding anomaly in the macroscopic quantities.
Let us focus on the new pressure-induced phase transition. As seen in Fig. 3 (a), above p ∼ 3.7
GPa, we observed a new resistance anomaly at T x (red arrows) below T N . This anomaly in ρ(T ) is
easily identified as a clear peak in dρ/dT as shown in Fig. 3 (b). Pressure dependence of T x is plotted
in Fig. 1 with closed (red) diamonds. The T x suddenly emerges above p ∼ 3.7 GPa, and strikingly

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JPS Conf. Proc. 3, 015044 (2014) 015044-5

8 2
p = 3.91 GPa (b)
(a) CeNiGe3
5.0 K 20
6 1.5 H // a p = 3.91 GPa
4.5 K I // c

dR/dH (mΩ/T)
R (mΩ)

µ0H (T)
4 1 TN
Tx
10 PM
4.5 K AFM
2 0.5 AFM I
II
5.0 K
0 0 0
0 5 10 0 2 4 6 8 10
µ0H (T) T (K)

Fig. 4. (a) Magnetic field dependence of the resistance (left axis) and the field differential of the resistance
(right axis) below T x at 3.91 GPa for H // a. (b) Temperature-magnetic field (T -H) phase diagram of CeNiGe3
at 3.91 GPa for H // a.

increases with increasing pressure. A magnetoresistance for H // a at 3.9 GPa exhibits a clear hys-
teresis anomaly below T x as shown in Fig. 4 (a), implying the first-order phase transition from new
pressure-induced phase to the low-pressure AFM phase (AFM-I). Both T N and T x is suppressed with
increasing magnetic field along the magnetic-easy axis, and the field dependences are summarized
in Fig. 4 (b). These experimental results indicate that the new pressure-induced phase above p ∼
3.7 GPa can be considered as an AFM phase (AFM-II) in which the magnetization, at least for H //
a-axis, is smaller than that of the AFM-I phase. Therefore, the new kink anomaly in ρ(T ) at T x is
associated with the successive phase transition from the AFM-I to the AFM-II.
Interestingly, the apparent SC transition simultaneously disappears with the emergence of the
AFM-II phase. These experimental facts demonstrate that the ordered state in the AFM-II phase
is conclusively different from the commensurate AFM-I state at lower pressures, because the low-
pressure SC state can only coexist with the commensurate AFM-I state, but not with the AFM-II state.
The longitudinal spin-density fluctuations which is observed in ref. [12] may possibly disappear in
the AFM-II phase, and the suppression of the longitudinal fluctuations may lead to the disappearance
of superconductivity in CeNiGe3 . Precise microscopic studies such as NMR/NQR and/or neutron
scattering experiments are required for better understanding of the AFM-II phase. High-pressure
experiments using a diamond anvil cell are now in progress to clarify the SC at higher pressures
properties in further detail.

4. Conclusion

The p-T phase diagram of CeNiGe3 was reinvestigated with the electrical resistivity measurement
using the single crystalline sample under the better hydrostatic condition up to p ∼ 4 GPa. We
discovered that the successive phase transition suddenly appears at T x above p ∼ 3.7 GPa, and the
pressure-induced SC phase disappears simultaneously. The application of magnetic field along the
a-axis suppresses the T x , indicating that the new phase can be considered as the antiferromagnetic
phase (AFM-II) with a small magnetization compared with the AFM-I phase at lower pressures. The
AFM-II phase is conclusively different from the commensurate AFM-I state, and the SC state can
coexist with the commensurate AFM-I phase, but not with the AFM II state.

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 Proceedings of the International Conference on Strongly Correlated Electron Systems (SCES2013)
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JPS Conf. Proc. 3, 015044 (2014) 015044-6

This work was supported by Grants-in-Aid for Scientific Research (No. 20340090) from Japan
Society for the Promotion of Science and a Grant-in-Aid for Scientific Research on Innovative Areas
”Heavy Electrons” (No. 21102513) of MEXT, Japan.

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