Superlattice formation lifting degeneracy protected by non-symmorphic symmetry through a metal-insulator transition in RuAs

The single crystal of RuAs obtained by Bi-flux method shows obvious successive metal-insulator transitions at T_MI1~255 K and T_MI2~195$ K. The X-ray diffraction measurement reveals a formation of superlattice of 3x3x3 of the original unit cell below T_MI2, accompanied by a change of the crystal system from the orthorhombic structure to the monoclinic one. Simple dimerization of the Ru ions is nor seen in the ground state. The multiple As sites observed in nuclear quadrupole resonance (NQR) spectrum also demonstrate the formation of the superlattice in the ground state, which is clarified to be nonmagnetic. The divergence in 1/T_1 at T_MI1 shows that a symmetry lowering by the metal-insulator transition is accompanied by strong critical fluctuations of some degrees of freedom. Using the structural parameters in the insulating state, the first principle calculation reproduces successfully the reasonable size of nuclear quadrupole frequencies for the multiple As sites, ensuring the high validity of the structural parameters. The calculation also gives a remarkable suppression in the density of states (DOS) near the Fermi level, although the gap opening is insufficient. A coupled modulation of the calculated Ru d electron numbers and the crystal structure proposes a formation of charge density wave (CDW) in RuAs. Some lacking factors remain, but it shows that a lifting of degeneracy protected by the non-symmorphic symmetry through the superlattice formation is a key ingredient for the metal-insulator transition in RuAs.Comment: 10 pages, 10 figure

Ferroic quadrupolar ordering in CeCoSi revealed using 59^{59}Co-NMR measurements

A nonmagnetic phase transition at $T_0 \sim 12$ K in the tetragonal system CeCoSi with a Kramers doublet ground state is reminiscent of an electric quadrupole ordering, even though its well-separated crystal-electric-field (CEF) levels are unlikely to acquire higher-order multipole degrees of freedom. Here, we report $^{59}$Co nuclear magnetic resonance (NMR) studies that are highly compatible with a ferroic quadrupole ordering below $T_0$. Changes in the NMR spectra below $T_0$ suggest that an external magnetic field induces ferroic Ce dipole moments orthogonal to the field, enabling domain selection in the nonmagnetic phase. Our findings suggest the presence of a ferroic $O_{zx}$-type quadrupole component in CeCoSi and demonstrate that quadrupole ordering may occur under well-separated CEF levels in tetragonal systems.Comment: 7 pages, 6 figures, 1 tabl