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Quasicrystal approximant (CexY1-x)Cd6 (0 < x < 1) forms a network of corner-sharing octahedra. We report that (Ce0.8Y0.2)Cd6 exhibits an anomalous magnetic transition which can be classified neither into the conventional static magnetic ordering nor into spin glasses. The anomalous transition is characterized by the coexistence of a static order and a frequency-dependent sharp positive anomaly in the 3rd-harmonic susceptibility. Based on the investigation of the reference systems CeCd6 and (Ce0.05Y0.95)Cd6, we speculate that the anomalous transition could be induced by disorder in the possible frustrated Ce-network in the presence of the Kondo effect., Comment: 5 figures

We have synthesized new Tsai-type Yb-based intermediate-valence approximant crystals (ACs) with different degree of approximation to quasicrystal, Zn--Au--Yb 1/1 and 2/1 AC, and studied the external pressure effect on their Yb mean-valence $\nu$. Whereas 1/1 AC distinctly exhibits a first-order-like jump in $\nu$ at a transition pressure $P_{\rm v}$, 2/1 AC only shows an indistinct anomaly at $P_{\rm v}$. We have also studied the pressure dependence of the $\nu$ of Au--Al--Yb 1/1 AC, which is a prototypal AC exhibiting pressure-induced quantum criticality. It shows a continuous valence anomaly at a critical pressure $P_{\rm c}$ where the magnetic susceptibility diverges toward zero temperature, in contrast to the valence jump in the Zn--Au--Yb 1/1 AC. These results are discussed based on a theoretical model of quantum critical valence fluctuation.

A strongly-correlated insulator, samarium mono-sulfide (SmS), presents not only the pressure-induced insulator-to-metal transition (IMT) with the color change from black to golden-yellow but also current-induced IMT (CIMT) with negative resistance. To clarify the origin of the CIMT of SmS, the electronic structure change has been investigated by optical reflectivity and angle-integrated photoelectron spectra by applying an electric current. At lower temperatures than about 100 K, where the nonlinear $V$-$I$ curve has been observed, the carrier density rapidly increases, accompanied by decreasing relaxation time of carriers with increasing current. Then, the direct gap size increases, and the mean valence changes from Sm$^{2+}$-dominant SmS to the mixed-valent one with increasing current. These results suggest that the CIMT originates from increasing the Sm $4f$-$5d$ hybridization intensity induced by the applied current., Comment: Main text: 6 pages, 4 figures, Supplementary materials: 2 pages, 2 figures

The photo-induced band structure variation of a rare-earth-based semiconductor, samarium monosulfide (SmS), was investigated using high-harmonic-generation laser-based time-resolved photoelectron spectroscopy. A nonlinear photo-induced band shift of the Sm 4f multiplets was observed. The first one is a shift to the high-binding-energy side due to a large surface photovoltage (SPV) effect of approximately 93 meV, comparable to the size of the bulk band gap, with a much longer relaxation time than 0.1 ms. The second one is an ultrafast band shift to the low binding energy side, which is in the opposite direction to the SPV shift, suggesting an ultrafast valence transition from divalent to trivalent Sm ions due to photo-excitation. The latter energy shift was approximately 58 meV, which is consistent with the energy gap shift from ambient pressure to the boundary between the black insulator and golden metallic phase with the application of pressure. This suggests that the photo-induced valence transition can reach the phase boundary, but other effects are necessary to realize the golden metallic phase., Comment: 6 pages, 4figures

The electronic structure changes of SmS surfaces under potassium (K) doping are elucidated using synchrotron-based core-level photoelectron spectroscopy and angle-resolved photoelectron spectroscopy (ARPES). The Sm core-level and ARPES spectra indicate that the Sm mean valence of the surface increased from the nearly divalent to trivalent states, with increasing K deposition. Carrier-induced valence transition (CIVT) from Sm$^{2+}$ to Sm$^{3+}$ exhibits a behavior opposite to that under conventional electron doping. Excess electrons are trapped by isolated excitons, which is inconsistent with the phase transition from the black insulator with Sm$^{2+}$ to the gold metal with Sm$^{3+}$ under pressure. This CIVT helps to clarify the pressure-induced black-to-golden phase transition in this material, which originates from the Mott transition of excitons., Comment: 7 pages, 6 figures

The phase separation of the ferromagnetic (FM) and paramagnetic (PM) phases in the superconducting (SC) state of UCoGe at the FM critical region was investigated using $^{59}$Co nuclear quadrupole resonance (NQR) technique by taking advantage of its site-selective feature. The NQR measurements revealed that the first-order quantum phase transition occurs between the FM and the PM states. The nuclear spin-lattice relaxation rate $1/T_1$ exhibited a clear drop at the SC state in the PM phase, whereas it was not detected in the FM phase, which indicates that the superconductivity in the FM phase becomes weaker at the FM critical region due to the presence of the PM SC state. This result suggests that the SC condensation energy of the PM SC state is equal or larger than that of the FM SC state in this region. The pressure-temperature phase diagram of UCoGe was modified by taking the results from this study into account., Comment: 4 pages, 4 figures

A $^{59}$Co nuclear magnetic resonance (NMR) measurement was performed on the single-crystalline ferromagnetic (FM) superconductor UCoGe under a pressure of 1.09 GPa, where the FM state is suppressed and superconductivity occurs in the paramagnetic (PM) state, to study the superconducting (SC) state in the PMstate. $^{59}$Co-NMR spectra became broader but hardly shifted across the SC transition temperature. The Knight-shift change determined from fitting the spectral peak with a Gaussian was much smaller than the spin part of the Knight shift; this is in good agreement with the spin-triplet pairing suggested from the large upper critical field. The spectrum broadening in the SC state cannot be attributed to the SC diamagnetic effect but is related to the properties of spin-triplet superconductivity. The origins of the broadening are discussed herein., Comment: 8 pages, 11 figures

A $^{59}$Co nuclear quadrupole resonance (NQR) was performed on a single-crystalline ferromagnetic (FM) superconductor UCoGe under pressure. The FM phase vanished at a critical pressure $P_c$, and the NQR spectrum just below $P_c$ showed phase separation of the FM and paramagnetic (PM) phases below Curie temperature $T_{\textrm{Curie}}$, suggesting first-order FM quantum phase transition (QPT). We found that the internal field was absent above $P_c$, but the superconductivity is almost unchanged. This result suggests the existence of the nonunitary to unitary transition of the superconductivity around $P_c$. Nuclear spin-lattice relaxation rate $1/T_1$ showed the FM critical fluctuations around $P_c$, which persist above $P_c$ and are clearly related to superconductivity in the PM phase. This FM QPT is understood to be a weak first order with critical fluctuations. $1/T_1$ sharply decreased in the superconducting (SC) state above $P_c$ with a single component, in contrast to the two-component $1/T_1$ in the FM SC state, indicating that the inhomogeneous SC state is a characteristic feature of the FM SC state in UCoGe., Comment: 5 pages, 4 figures

The hexagonal ZrNiAl-type (space group: P-62m) and the tetragonal Mo2FeB2-type (space group: P4/mbm) structures, which are frequently formed in the same Yb-based alloys and exhibit physical properties related to valence-fluctuation, can be regarded as approximants of a hypothetical dodecagonal quasicrystal. Using Pd-Sn-Yb system as an example, a model of quasicrystal structure has been constructed, of which 5-dimensional crystal (space group: P12/mmm, aDD=5.66 {\AA} and c=3.72 {\AA}) consists of four types of acceptance regions located at the following crystallographic sites; Yb [00000], Pd[1/3 0 1/3 0 1/2], Pd[1/3 1/3 1/3 1/3 0] and Sn[1/2 00 1/2 1/2]. In the 3-dimensional space, the quasicrystal is composed of three types of columns, of which c-projections correspond to a square, an equilateral triangle and a 3-fold hexagon. They are fragments of two known crystals, the hexagonal {\alpha}-YbPdSn and the tetragonal Yb2Pd2Sn structures. The model of the hypothetical quasicrystal may be applicable as a platform to treat in a unified manner the heavy fermion properties in the two types of Yb-based crystals., Comment: 19 pages, 6 figures

We have performed $^{27}$Al-NMR measurements on single-crystalline UPd$_2$Al$_3$ with the field parallel to the $c$ axis to investigate the superconducting (SC) properties near the upper critical field of superconductivity $H_{\rm c2}$. The broadening of the NMR linewidth below 14~K indicates the appearance of the internal field at the Al site, which originates from the antiferromagnetically ordered moments of U 5$f$ electrons. In the SC state well below $\mu_0H_{\rm c2}$ = 3.4~T, the broadening of the NMR linewidth due to the SC diamagnetism and a decrease in the Knight shift are observed, which are well-understood by the framework of spin-singlet superconductivity. In contrast, the Knight shift does not change below $T_{\rm c}(H)$, and the NMR spectrum is broadened symmetrically in the SC state in the field range of 3~T $< \mu_0 H < \mu_0 H_{\rm c2}$. The unusual NMR spectrum near $H_{\rm c2}$ suggests that a spatially inhomogeneous SC state such as the Fulde-Ferrell-Larkin-Ovchinnikov (FFLO) state would be realized., Comment: 5 pages, 5 figures

We report on ac magnetic susceptibility measurements under pressure of the Au-Al-Yb alloy, a crystalline approximant to the icosahedral quasicrystal that shows unconventional quantum criticality. In describing the susceptibility as $\chi(T)^{-1} - \chi(0)^{-1} \propto T^{\gamma}$, we find that $\chi(0)^{-1}$ decreases with increasing pressure and vanishes to zero at the critical pressure $P_{\rm c} \simeq 2$ GPa, with $\gamma~ (\simeq 0.5)$ unchanged. We suggest that this quantum criticality emerges owing to critical valence fluctuations. Above $P_{\rm c}$, the approximant undergoes a magnetic transition at $T \simeq 100$ mK. These results are contrasted with the fact that, in the quasicrystal, the quantum criticality is robust against the application of pressure. The applicability of the so-called $T/H$ scaling to the approximant is also discussed., Comment: 11 pages, 5 figures

We report the synthesis of a single-phase sample of the superconducting crystalline approximant Au64.0Ge22.0Yb14.0 and present a structure model refined by Rietveld analysis for X-ray diffraction data., Comment: 3 pages, 3 figures, http://dx.doi.org/10.7566/JPSJ.84.015002

We report the emergence of bulk superconductivity in Au64.0Ge22.0Yb14.0 and Au63.5Ge20.5Yb16.0 below 0.68 and 0.36 K, respectively. This is the first observation of superconductivity in Tsai-type crystalline approximants of quasicrystals. The Tsai-type cluster center is occupied by Au and Ge ions in the former approximant, and by an Yb ion in the latter. For magnetism, the latter system shows a larger magnetization than the former. To explain this observation, we propose a model that the cluster-center Yb ion is magnetic. The relationship between the magnetism and the superconductivity is also discussed., Comment: 5 pages, 4 figures, http://dx.doi.org/10.7566/JPSJ.84.023705

We have performed 59Co NMR experiments on the ferromagnetic superconductor UCoGe under magnetic fields (H) along the a- and b- axes to investigate the relationship between ferromagnetic properties and superconductivity. The ferromagnetic ordering temperature TCurie is suppressed and the nuclear spin-lattice relaxation rate 1/T1 at 2 K is enhanced in H || b, although TCurie and 1/T1 are unchanged in H || a, indicating that the ferromagnetic criticality is induced only when H is applied along the b axis. We show the close relationship between the magnetic anisotropies and the superconducting ones reported by Aoki et al.: the superconductivity is gradually suppressed in H || a, but enhanced in H || b above 5 T. We strongly suggest that the enhancement of the superconductivity observed in H || b originates from the field induced ferromagnetic criticality, as pointed out by Aoki et al and Mineev., Comment: 5 pages, 5 figures, to appear in J. Phys. Soc. Jpn

Quantum criticality has been considered to be specific to crystalline materials such as heavy fermions. Very recently, however, the Tsai-type quasicrystal Au51Al34Yb15 has been reported to show unusual quantum critical behavior. To obtain a deeper understanding of this new material, we have searched for other Tsai-type cluster materials. Here, we report that the metal alloys Au44Ga41Yb15 and Ag47Ga38Yb15 are members of the 1/1 approximant to the Tsai-type quasicrystal and that both possess no localized magnetic moment. We suggest that the Au-Al-Yb system is located near the border of the divalent and trivalent states of the Yb ion; we also discuss a possible origin of the disappearance of magnetism, associated with the valence change, by the substitution of the constituent elements., Comment: 21 pages, 6 figures, http://dx.doi.org/10.7566/JPSJ.83.034705

The temperature, field, and field-orientation dependences of the electronic specific heat Ce of the ironpnictide superconductor KFe2As2 have been investigated. Thermodynamic evidence of the presence of line nodes is obtained from the T and $\sqrt{H}$ linear dependences of Ce/T in the low-T and low-H region. Under a magnetic field rotated within the tetragonal ab plane, a fourfold oscillation is observed in Ce with a sign change at 0.08Tc. On the basis of the Doppler-shift analysis, the observed Ce minima in H // [100] at low T indicate the presence of line nodes somewhere on the Fermi surface where the Fermi velocity is parallel to the [100] direction; this is consistent with the octet-line-node scenario proposed recently by a photoemission experiment. In addition, the low-T Ce/T exhibits an unusual upturn on cooling at moderate fields only for H // ab, which is understood in terms of the strong Pauli paramagnetic effect on multiband superconductivity., Comment: 4 pages, 4 figures, published in J. Phys. Soc. Jpn

The low-temperature magnetic properties of LaCoGe with the tetragonal CeFeSi-type structure were investigated by ^{59}Co- and ^{139}La-nuclear magnetic resonance (NMR) and nuclear quadrupole resonance (NQR) measurements. The nuclear spin-lattice relaxation rate divided by the temperature, 1/(T_1 T), gradually increases with decreasing temperature and shows a kink at approximately 18 K, below which an inhomogeneous internal field appears at the Co nuclear site. These results indicate that antiferromagnetic ordering occurs below T_N ~ 18 K. However, an internal field was not observed at the La nuclear site below T_N. Taking all NMR results into account, we conclude that spin-density-wave (SDW)-type ordering occurs, where magnetic correlations are of the checkerboard type in the ab-plane and have a long periodicity along the c-axis with inhomogeneous ordered moments pointing to the c-axis.

Quasicrystals are metallic alloys that possess long-range, aperiodic structures with diffraction symmetries forbidden to conventional crystals. Since the discovery of quasicrystals by Schechtman et al. at 1984 (ref. 1), there has been considerable progress in resolving their geometric structure. For example, it is well known that the golden ratio of mathematics and art occurs over and over again in their crystal structure. However, the characteristic properties of the electronic states - whether they are extended as in periodic crystals or localized as in amorphous materials - are still unresolved. Here we report the first observation of quantum (T = 0) critical phenomena of the Au-Al-Yb quasicrystal - the magnetic susceptibility and the electronic specific heat coefficient arising from strongly correlated 4f electrons of the Yb atoms diverge as T -> 0. Furthermore, we observe that this quantum critical phenomenon is robust against hydrostatic pressure. By contrast, there is no such divergence in a crystalline approximant, a phase whose composition is close to that of the quasicrystal and whose unit cell has atomic decorations (that is, icosahedral clusters of atoms) that look like the quasicrystal. These results clearly indicate that the quantum criticality is associated with the unique electronic state of the quasicrystal, that is, a spatially confined critical state. Finally we discuss the possibility that there is a general law underlying the conventional crystals and the quasicrystals., Comment: 21 pages, 6 figures, http://www.nature.com/nmat/journal/vaop/ncurrent/full/nmat3432.html

Golden SmS is a paramagnetic, mixed-valence system with a pseudogap. With increasing pressure across a critical pressure Pc, the system undergoes a discontinuous transition into a metallic, anti-ferromagnetically ordered state. By using a combination of thermodynamic, transport, and magnetic measurements, we show that the pseudogap results from the formation of a local bound state with spin singlet. We further argue that the transition Pc is regarded as a transition from an insulating electron-hole gas to a Kondo metal, i.e., from a spatially bound state to a Kondo virtually bound state between 4f and conduction electrons., Comment: 5 pages, 5 figures

We have performed ^{59}Co-nuclear quadrupole resonance (NQR) and nuclear magnetic resonance (NMR) studies on YCoGe, which is a reference compound of ferromagnetic superconductor UCoGe, in order to investigate the magnetic properties at the Co site. Magnetic and superconducting transitions were not observed down to 0.3 K, but a conventional metallic behavior was found in YCoGe, although its crystal structure is similar to that of UCoGe. From the comparison between experimental results of two compounds, the ferromagnetism and superconductivity observed in UCoGe originate from the U-5f electrons., Comment: 4 pages, 6 figures, accepted for JPSJ

We report ac magnetic susceptibility and dc magnetization measurements on the superconducting ferromagnet UCoGe (with superconducting and Curie temperatures of $T_{{\rm SC}} \sim 0.5$~K and $T_{{\rm Curie}} \sim 2.5$~K, respectively). In the normal, ferromagnetic state ($T_{{\rm SC}} < T < T_{{\rm Curie}}$), the magnetization curve exhibits a hysteresis loop similar to that of a regular itinerant ferromagnet. Upon lowering the temperature below $T_{{\rm SC}}$, the spontaneous magnetization is unchanged, but the hysteresis is markedly enhanced. Even deeply inside the superconducting state, ferromagnetism is not completely shielded, and there is no Meissner region, a magnetic field region of $H < H_{\rm c1}$ (a lower critical field). From these results, we suggest that UCoGe is the first material in which ferromagnetism robustly survives in the superconducting state and a spontaneous vortex state without the Meissner state is realized., Comment: 5 pages, 4 figures, to be published in J. Phys. Soc. Jpn

Unambiguous evidence for the microscopic coexistence of ferromagnetism and superconductivity in UCoGe ($T_{\rm Curie} \sim 2.5$ K and $T_{\rm SC}$ $\sim$ 0.6 K) is reported from $^{59}$Co nuclear quadrupole resonance (NQR). The $^{59}$Co-NQR signal below 1 K indicates ferromagnetism throughout the sample volume, while nuclear spin-lattice relaxation rate $1/T_1$ in the ferromagnetic (FM) phase decreases below $T_{\rm SC}$ due to the opening of the superconducting(SC) gap. The SC state was found to be inhomogeneous, suggestive of a self-induced vortex state, potentially realizable in a FM superconductor. In addition, the $^{59}$Co-NQR spectrum around $T_{\rm Curie}$ show that the FM transition in UCoGe possesses a first-order character, which is consistent with the theoretical prediction that the low-temperature FM transition in itinerant magnets is generically of first-order., Comment: 5 pages, 5 figures

We measured the thermal expansion of the valence fluctuating phase of SmS (golden SmS) to construct a pressure vs temperature phase diagram. The obtained phase diagram is characterized by three lines. One is a crossover line that divides the paramagnetic phase into two regions. The other two lines correspond to a second-order Neel transition and a first-order Neel transition. The crossover line appears to emerge from a tricritical point that separates the first-order Neel transition from the second-order one. We argue that a valence jump occurs at the border of antiferromagnetism., Comment: 5 pages, 5 figures

Co nuclear magnetic resonance (NMR) and nuclear quadrupole resonance (NQR) studies were performed in the recently discovered UCoGe, in which the ferromagnetic and superconducting (SC) transitions were reported to occur at $T_{\rm Curie} \sim 3$ K and $T_S \sim 0.8$ K (N. T. Huy {\it et al.}, Phys. Rev. Lett. {\bf 99} (2007) 067006), in order to investigate the coexistence of ferromagnetism and superconductivity as well as the normal-state and SC properties from a microscopic point of view. From the nuclear spin-lattice relaxation rate $1/T_1$ and Knight-shift measurements, we confirmed that ferromagnetic fluctuations which possess a quantum critical character are present above $T_{\rm Curie}$ and the occurrence of ferromagnetic transition at 2.5 K in our polycrystalline sample. The magnetic fluctuations in the normal state show that UCoGe is an itinerant ferromagnet similar to ZrZn$_2$ and YCo$_2$. The onset SC transition was identified at $T_S \sim 0.7$ K, below which $1/T_1$ of 30 % of the volume fraction starts to decrease due to the opening of the SC gap. This component of $1/T_1$, which follows a $T^3$ dependence in the temperature range of $0.3 - 0.1$ K, coexists with the magnetic components of $1/T_1$ showing a $\sqrt{T}$ dependence below $T_S$. From the NQR measurements in the SC state, we suggest that the self-induced vortex state is realized in UCoGe., Comment: 5 pages, 7 figures. submitted to J. Phys. Soc. Jpn. To appear in J. Phys. Soc. Jpn