Journal of the Physical Society of Japan

Vol. 77, No. 6, June, 2008, 063706

#2008 The Physical Society of Japan LETTERS

Magnetic Excitations in Heavy Electron State of Filled

Skutterudite Prx La1x Fe4 P12 (x ¼ 1:00 and 0.85)
Kazuaki I WASA, Lijie H AO, Tomoo HASEGAWAy, Kenji H ORIUCHIz,
Youichi M URAKAMI, Junya OTSUKI, Yoshio K URAMOTO, Masahumi K OHGI1 ,
Keitaro K UWAHARA1 x, Hitoshi SUGAWARA2 , Yuji A OKI1 , and Hideyuki S ATO1
Department of Physics, Tohoku University, Sendai 980-8578
1
Department of Physics, Tokyo Metropolitan University, Hachioji, Tokyo 192-0397
2
Department of Mathematical and Natural Sciences, The University of Tokushima, Tokushima 770-8502
(Received April 3, 2008; accepted April 15, 2008; published May 26, 2008)
PrFe4 P12 exhibits clear heavy electron behaviors as well as the phase transition to an antiferro-type
ordering of 4f electron state. In this paper, we report on inelastic neutron scattering results for powdered
samples of Prx La1x Fe4 P12 (x ¼ 1:00 and 0.85). A clear quasielastic magnetic response is observed, and
no distinct signal is seen for crystal-field (CF) excitations in the heavy electron state. A model with
strong hybridization between conduction electrons and Pr3þ 4f 2 electrons [J. Otsuki et al.: J. Phys. Soc.
Jpn. 74 (2005) 200 and 2082] is consistent with the observed magnetic response. This result shows that
the heavy electron behavior of Prx La1x Fe4 P12 (x ¼ 1:00 and 0.85) originates from the Kondo effect
associated with low-lying singlet–triplet CF states.

KEYWORDS: heavy electron, rare-earth filled skutterudite, neutron scattering, dynamical magnetic susceptibility
DOI: 10.1143/JPSJ.77.063706

The heavy electron state in the system with two or more
4f electrons per rare-earth ion has been actively studied
recently, after numerous studies on Ce-based compounds
with one 4f electron per Ce ion.1) For example, PrInAg2 is a
typical heavy electron material, whose specific heat coef-
ficient takes a huge value of 6.5 J/(molK2 ) at low temper-
atures.2) PrPb3 and the systems diluted by La substitution
also exhibit an enhancement of electronic mass, as observed
in the specific heat.3) These materials have been studied as
candidates for the quadrupolar Kondo effect due to a non-
Kramers doublet crystal-field (CF) ground state.
The rare-earth filled skutterudite compounds RT4 X12
(R = rare earth, T = transition metal, X = pnictogen)
crystallizing in an Im3 cubic structure are ideal systems
for studying various physical properties.4,5) For example,
PrOs4 Sb12 is famous for its superconductivity due to heavy
quasiparticles deduced from the huge jump of the specific
heat at the transition temperature TC ¼ 1:85 K.6) NdFe4 P12
exhibits the  log T dependence of electrical resistivity
between 4 and 15 K, in contrast to the distinct ferromagnetic
ordering at 1.9 K.7) SmOs4 Sb12 shows a heavy electron state
being robust against a magnetic field.8,9) In this paper, we
focus on PrFe4 P12 . Before describing the heavy electron
properties of this material, its phase transition should
be mentioned briefly. The low-temperature phase below
TA ¼ 6:5 K at zero magnetic field has been found to be
nonmagnetic, since neutron diffraction10) and SR11) experi-
studies for single crystalline samples revealed an antiferro-
magnetic component with the same q0 , induced by an
applied magnetic field in the low-temperature phase.14,15)
These experimental findings indicate the antiferro-type
ordering of Pr3þ ion 4f 2 electron multipoles. Recently, a
scalar-type (1 -type) order parameter has been suggest-
ed;16,17) this is analogous to the order parameter below the
metal–nonmetal transition of PrRu4 P12 .18,19)
In the region where the ordered phase is destroyed by
external magnetic fields of 4 – 7 T, the electronic specific
heat coefficient for the T-linear term becomes as large
as 1.4 J/(molK2 ).20) A cyclotron effective mass up to 81m0
has been detected in a de Haas–van Alphen effect experi-
ment.21) The electrical resistivity behaves as  log T be-
tween 30 and 100 K. These phenomena can be attributed
to the Kondo effect. Hereafter, we concentrate on the
dynamical properties of heavy electrons in PrFe4 P12 . The
31
P-NMR study on the temperature variation of nuclear spin-
lattice relaxation rate in PrFe4 P12 also suggested the Kondo
effect.22)
Recently, Otsuki and coworkers provided a theoretical
scenario for heavy electrons in the Pr-based skutterudite
based on the p– f hybridization effect between 4f and
conduction electrons originating from pnictogen orbitals
with au symmetry.23,24) Under the Th point group of
skutterudites, the J ¼ 4 multiplet of 4f 2 states splits into a
singlet 1 , a doublet 23 , and two triplets ð1Þ
4 and 4 .
ð2Þ 25)

ments did not reveal any magnetic signal. X-ray diffraction
experiment revealed a structural superlattice characterized
by the wave vector q0 ¼ ð1; 0; 0Þ below TA .12) The Fermi-
surface nesting condition with this wave vector is predicted
in a band calculation.13) Moreover, neutron diffraction

E-mail: iwasa@iiyo.phys.tohoku.ac.jp
y
Present address: Bridgestone Corporation, Kodaira, Tokyo 187-8531.
z
Present address: The Yokohama Rubber Co., Ltd., Hiratsuka, Kanagawa
254-8601.
x
Present address: Institute of Applied Beam Science, Ibaraki University,
Mito 310-8512.
063706-1
The triplets can be expressed as linear combinations of 4
and 5 for Oh symmetry. Considering the low-energy quasi-
quartet scheme composed of a singlet and a triplet and
hybridization effects in the Pr-based skutterudite, they
derived an antiferromagnetic exchange coupling between
4f and conduction electrons. This theoretical argument
suggested that the Kondo effect is responsible for the heavy
electron state in the 4f 2 systems. On the basis of this
scenario, they derived a dynamical magnetic susceptibility.
This result should be directly compared with the magnetic
excitation spectrum obtained by neutron scattering.
J. Phys. Soc. Jpn., Vol. 77, No. 6 LETTERS K. IWASA et al.

0.06 0.06
PrFe4P12 T = 60 K Pr0.85La0.15Fe4P12 T = 50 K
0.04 0.04

0.02 0.02

0.00 0.00

S (E) [barn / meV / sr / Pr]

S(E) [barn / meV / sr / Pr]

0.06 0.06
T = 15 K T = 25 K
0.04 0.04

0.02 0.02

0.00 0.00

0.06 0.06
observed
observed T = 1.5 K
T = 6.7 K 0.04 fitted
0.04 fitted

0.02 0.02

0.00 0.00
0 5 10 15 20 0 5 10 15 20
Energy [meV]
Energy [meV]
Fig. 2. Open circles represent the scattering function of the powdered
Fig. 1. Open circles represent the scattering function of the powdered
sample of Pr0:85 La0:15 Fe4 P12 . Solid lines indicate results of the least-
sample of PrFe4 P12 . Solid lines indicate results of the least-squares fitting
squares fitting procedure based on eqs. (1) and (2).
procedure based on eqs. (1) and (2).

The La-substituted compound by 15% to Pr-ion sites of
PrFe4 P12 does not undergo the low-temperature phase
transition, and the large specific heat coefficient persists
down to the lowest temperature.26) This fact is understood
as the stabilization of the low-lying Kondo state by the
suppression of the long-range nonmagnetic order due to the
disruption of interactions between Pr ions.
To investigate experimentally the 4f electron contribution
to the heavy electron state, we performed inelastic neutron
scattering on Prx La1x Fe4 P12 (x ¼ 1:00 and 0.85) and
examined the aforementioned theory. A part of this study
has been published elsewhere.27–29)
Single crystals of Prx La1x Fe4 P12 (x ¼ 1:00, 0.85, and
0.00) were synthesized by the Sn-flux method, as described
previously.4) Neutron inelastic scattering experiments for
powdered samples from these single crystals were carried
out at the time-of-flight spectrometer LAM-D with large
focus analyzer mirrors installed in the pulsed neutron facility
KENS, KEK, Tsukuba (Japan). The final neutron energy was
selected as 4.593 meV, and the energy resolution, 350 meV at
the elastic scattering position. The sample temperatures were
controlled with a liquid helium cryostat or a helium-gas
closed-cycle refrigerator.
Figure 1 shows the measured scattering function SðEÞ as a
function of excitation energy E above TA of PrFe4 P12 . This
result was obtained after the normalization of scattered
intensity using the energy dependence of incident neutron
intensity and subtractions of backgrounds estimated from
the measurements without the samples, as well as phonon
contributions estimated from the measurement of LaFe4 P12 .
The intensities were transformed into the absolute values
of the scattering cross section using the incoherent scat-
tering intensity from the standard vanadium sample. We
observed quasielastic spectra whose widths are much larger
than the energy resolution. A similar quasielastic magnetic
response is observed in the SðEÞ of Pr0:85 La0:15 Fe4 P12 down
to 1.5 K, as shown in Fig. 2. For both compounds, no CF
063706-2
excitation peak was observed in the range up to 100 meV,
indicating the strong hybridization between 4f and con-
duction electrons. One can expect that the 4f electron CF
excited states will be located in the energy range less than
5 meV, as seen in the width of the quasielastic spectra at
1.5 K.
To derive experimentally the imaginary part 00 ðEÞ of the
dynamical magnetic susceptibility, the following equation
with a Lorentzian function was adopted for analysis.
1 2 00
SðEÞ ¼ r02 fmag
2
ðnðEÞ þ 1Þ 2
 ðEÞ ð1Þ
ðgB Þ 3
ð0Þ E
00 ðEÞ ¼ 2 ð2Þ
E þ 2
Here, r0 ¼ 0:539  1012 cm, fmag is the magnetic form
factor of Pr3þ , B is the Bohr magneton, and nðEÞ represents
the Bose–Einstein distribution function. The spectrum of a
heavy electron system might be composed of a quasielastic
component and inelastic peaks of CF excitations. Within the
present experimental accuracy, the quasielastic and inelastic
components cannot be dissolved. Therefore, we adopted the
simple form of 00 ðEÞ expressed by eq. (2). The validity of
this analysis will be discussed in the comparison with the
theoretical result. Least-squares fitting was performed using
this spectral form with the free parameters ð0Þ and  . The
instrumental resolution is convoluted for the data except for
the incoherent scattering contribution around E ¼ 0. The
results shown by lines in Figs. 1 and 2 reproduce satisfac-
torily the experimental data. The  and ð0Þ obtained as
functions of temperature are shown in Fig. 3. The  shown
in Fig. 3(a) exhibits a monotonic increase with increasing
temperature, as observed in typical heavy electron systems.
The ð0Þ shown in Fig. 3(b) increases with a decrease in
temperature and exhibits a saturating behavior at the lowest
temperature of the disordered state. Such a behavior is
similar to the Pauli paramagnetic feature of the typical heavy
electron systems.
J. Phys. Soc. Jpn., Vol. 77, No. 6 LETTERS K. IWASA et al.

60 electrons. On the other hand, PrOs4 Sb12 and PrRu4 Sb12

(a) exhibit well-defined CF peaks (less hybridization) owing to
50 PrFe4P12 the low-lying scheme of 1 and ð2Þ 4 that is dominantly
Pr0.85La0.15Fe4P12 composed of 5 . This is consistent with the theoretical result
40 1/2
fitted (T ) indicating that the 5 excited state does not contribute to
Γ [K]

30 the Kondo effect. Therefore, the low-energy scheme in

20
Prx La1x Fe4 P12 is dominated by the 4 characteristic. This
inference for the low-energy scheme was also given by the
10 NCA analysis of magnetization anisotropy.20)
(J1ρc = 0.22, ΔCF = 22 K)
The temperature
pffiffiffiffi dependence of  is close to a function
0
0 10 20 30 40 50 60 70 proportional to T , as shown by a broken line in Fig. 3(a).
This feature has often been observed in typical heavy
Temperature [K]
fermion compounds, but it is not sufficient to conclude the
Kondo effect with the expected low-lying CF state. To
(b) discuss this in detail, we examined the theory based on the
0.3 PrFe4P12 non-crossing approximation (NCA) considering the expect-
χ (0)/(gμB) [K ]

Pr0.85La0.15Fe4P12
-1

ed low-lying CF levels. The present measurements were

0.2 carried out for the powdered sample with the wide-area
2

neutron analyzer mirrors. This condition yielded the average

0.1 NCA
(J1ρc = 0.22)
(ΔCF = 22 K)
0.0
0 1
10 10
Temperature [K]
Fig. 3. Symbols represent the (a)  and (b) ð0Þ of PrFe4 P12 and
Pr0:85 La0:15 Fe4 P12 determined from the present neutron scattering
measurements. Solid lines indicate the NCA results for J1 c ¼ 0:22
and the bare CF splitting CF ¼ 22 K between the singlet and triplet
states. A broken line represents
pffiffiffiffi the result of least-squares fitting of a
function proportional to T to the data points of the  of PrFe4 P12 and
Pr0:85 La0:15 Fe4 P12 .
To understand the overdamped magnetic excitation
spectra in Prx La1x Fe4 P12 , we first discuss the CF scheme
by comparing it with those of other Pr-filled skutterudite
compounds. PrRu4 P12 , which exhibits a metal–nonmetal
phase transition at TM{I ¼ 63 K, has a 1 singlet ground state
above TM{I [1 (0 meV)–ð1Þ ð2Þ
4 (5.87 meV)–4 (10.83 meV)–
23 (13.27 meV)]. This compound exhibits a very broad
magnetic spectrum near TM{I as in the case of Prx La1x -
Fe4 P12 , while the CF excitations become sharp and their
levels depend on temperature below TM{I .30) The scheme
of the superconductor PrOs4 Sb12 is 1 (0 meV)–ð2Þ 4 determined by the analysis of the dynamical data. Note that
(0.68 meV)–ð1Þ4 (11.6 meV)–23 (17.7 meV).
31,32)
Although
the peaks of CF excitations in neutron scattering spectra
become slightly broader with increasing temperature through
TC , the well-defined peaks are observed in the entire
temperature range, in contrast to the present result for
Prx La1x Fe4 P12 . PrRu4 Sb12 has the scheme 1 (0 meV)–ð2Þ 4
(5.26 meV)–ð1Þ4 (11.83 meV)–23 (15.79 meV),33) and its
spectrum is composed of much sharper peaks than the
quasielastic response of Prx La1x Fe4 P12 .
The possible origin of the heavy electron behavior in
Prx La1x Fe4 P12 has been discussed theoretically.23,24) The
authors considered the scheme with the singlet ground state
1 and the excited triplets 4 or 5 . The scheme with the 4
excited state gives rise to an antiferromagnetic c– f exchange
interaction, which causes the Kondo effect producing heavy
magnetic response over the reciprocal space (Brillouin
zone), and the data was regarded as the Pr-ion single-site
response. Thus, we directly compared the experimental
result with the NCA calculation of 00 ðEÞ for the single-site
2 Pr-ion state. The parameters in the NCA calculation are the
10
product of the antiferromagnetic exchange coupling J1 and
the conduction electron density of states c , as well as
the splitting energy CF between the singlet and triplet
states. We chose J1 c ¼ 0:22 and the bare CF splitting
CF ¼ 22 K. The magnitude of J1 c should be sufficiently
large to produce the dominant quasielastic response, as seen
in Fig. 10(b) of ref. 24 that is consistent with the present
analysis result based on eq. (2). The calculated result for 
is shown by the solid line in Fig. 3(a), where the low-
temperature magnitudes of the calculated and experimental-
ly determined spectral widths  become close to each other.
It should be mentioned that CF is renormalized to be about
10 K by the interaction with conduction electrons, and the
results are insensitive to the choice of smaller CF . The
overall feature of monotonic increase obtained by reducing
T together with a steep variation in the lower T region well
reproduces the experimental features. The discrepancy
observed in the higher temperature range may partly be
due to contributions of higher-energy CF levels, which were
not considered in the calculation.
Figure 3(b) shows the static magnetic susceptibility
the experimental susceptibility is not for the response against
a homogeneous magnetic field, but for the local response
mentioned above. The solid line in Fig. 3(b) shows the
calculated result for ð0Þ against temperature with the same
values of J1 c and CF as those in Fig. 3(a). The data point
at 1.5 K of Pr0:85 La0:15 Fe4 P12 is very close to the NCA
calculation. Since 00 ðEÞ at this low temperature should be
dominated by the lower singlet–triplet levels, the good
agreement is reasonable. Namely, the experimentally deter-
mined  and ð0Þ of Prx La1x Fe4 P12 at the lowest temper-
ature are reproduced well by the NCA calculation. We
emphasize that the value (0.22) of the exchange coupling
J1 c is of central importance, and the value of CF is not
crucial as long as it is about 22 K or smaller. In this sense, no
free parameters have been left in fitting ð0Þ. This indicates
063706-3
J. Phys. Soc. Jpn., Vol. 77, No. 6 LETTERS
that the heavy electron and strongly hybridized state in this
system are attributed to the Kondo effect within the quasi-
quartet CF scheme involving the triplet ð1Þ
4 dominated by 4
in the Oh symmetry. The larger experimental value of ð0Þ
than that in the NCA at high temperatures may be due to the
contribution of the excited levels located above the singlet–
triplet states, as in the case of  . In addition, we cannot
exclude the possibility that the impurity model assumed in
the NCA is insufficient for the quantitative analysis of the
temperature variation.
In conclusion, the present neutron inelastic scattering
study of PrFe4 P12 and Pr0:85 La0:15 Fe4 P12 in their heavy
electron states elucidates the quasielastic magnetic response.
The observed spectra are in good agreement with the
dynamical magnetic susceptibility calculated with the anti-
ferromagnetic coupling between conduction and Pr3þ 4f 2
electrons. Thus, the heavy electron state should originate
from the Kondo effect. The present results also give the basis
for understanding the nonmagnetic ordering below TA whose
order parameter is expected to be a scalar-type (1 -type)
one.16,17)
Acknowledgment
Professor J.-G. Park is acknowledged for his valuable
discussion on the neutron scattering data. This study is
supported in part by Grants-in-Aid for Scientific Research
(Nos. 15072206, 15740219, and 1604659) from the Min-
istry of Education, Culture, Sports, Science and Technology,
Japan and Yamada Science Foundation. The neutron
scattering experiments were performed under the User
Program conducted by KENS, KEK. One of the authors
(L.H.) thanks the Japan Society for the Promotion of Science
(JSPS) for the financial support provided to her as a JSPS
Fellow.
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