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Systematic research was performed to investigate magnetic properties of the Tsai-type Ga-Pd-RE (RE = Gd, Tb, Dy, and Ho) systems, where both 1/1 and 2/1 quasicrystal approximants (ACs) are attainable at the same compositions as thermodynamical stable phases. Most of the samples exhibited spin-glass (SG)-like freezing behavior at low temperatures except Ga-Pd-Tb 2/1 AC and Ga-Pd-Ho 1/1 AC. The former showcased antiferromagnetic order at 5.78 K while the latter did not show any anomaly down to 1.8 K. Furthermore, 2/1 ACs were noticed to be less frustrated than their corresponding 1/1 ACs presumably due to the disorder-free environment in the nearest neighbors of the rare earth sites that form a network of distorted octahedron in the 2/1 ACs. The spin dynamic in SG samples was also characterized by means of ac magnetic susceptibility measurements. The results evidenced a weak response of the freezing temperatures to the measurement frequency in the Heisenberg systems, i.e., Gd-contained ACs, in contrast to the non-Heisenberg systems, i.e., Tb, Dy and Ho-contained ACs, where significant dependency is noticed for the latter. The spin-glass samples were further examined by fitting their freezing temperatures to the Vogel-Fulcher law.

The atomic structure of the recently discovered antiferromagnetic Ga50Pd35.5Tb14.5 2/1 approximant to quasicrystal with the space group of Pa-3(No. 205), a = 23.1449(0) angstrom was determined by means of a single crystal X-ray diffraction. The refined structure model revealed two main building units, namely, a Tsai-type rhombic triacontahedron (RTH) cluster with three concentric inner shells and an acute rhombohedron filling the gaps in between the RTH clusters. One of the interesting findings was a very low number of chemically mixed sites in the structure, which amount to only 7.40 % of the all the atomic sites within an RTH cluster. In particular, a disorder-free environment was noticed within a nearest neighbor of an isolated Tb3+ ion, which is presumably one of the main contributors in enhancing antiferromagnetic order in the present compound. The second significant finding was the observance of an orientationally ordered trigonal pyramid-like unit with a height of 4.2441(7) angstrom at the center of the RTH cluster, which has never been observed in Tsai-type compounds before. Such unit is noticed to bring structural distortion to outer shells, in particular, to the surrounding dodecahedron cage being another possible contributor of the antiferromagnetic order establishment in the present compound. The results, therefore, are suggestive of a possible link between chemical/positional order and the antiferromagnetic order establishment.

Magnetic properties of the quasicrystal approximant Au$_{65}$Ga$_{21}$Tb$_{14}$ were investigated by the magnetization and the neutron diffraction experiments. The temperature dependences of the magnetic susceptibility and the magnetization curve indicate dominant ferromagnetic interactions, while the whirling antiferromagnetic order was found from the neutron diffraction experiments. In the antiferromagnetic phase, the magnetic moments are aligned almost perpendicular to a pseudo five-fold symmetry axis, which should correspond to the easy-axis direction of a Tb atom. The magnetic properties similar to those of Au$_{72}$Al$_{14}$Tb$_{14}$ in spite of the difference in the electron-per-atom ratio suggest the robustness of the easy-axis anisotropy against the chemical substitution of the nonmagnetic atoms., Comment: 6 pages, 3 figures, 2 tables

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

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