Negative volume thermal expansion via orbital and magnetic orders in Ca2Ru1-(x)Cr(x)O4(0 < x < 0.13).

Ca2RuO4 undergoes a metal-insulator transition at T(MI)=357 K, followed by a well-separated transition to antiferromagnetic order at T(N)=110 K. Dilute Cr doping for Ru reduces the temperature of the orthorhombic distortion at T(MI) and induces ferromagnetic behavior at T(C). The lattice volume V of Ca2Ru1-(x)Cr(x)O4 (0 < x < 0.13) abruptly expands with cooling at both T(MI) and T(C), giving rise to a total volume expansion ΔV/V ≈ 1%, which sharply contrasts the smooth temperature dependence of the few known examples of negative volume thermal expansion driven by anharmonic phonon modes. In addition, the near absence of volume thermal expansion between T(C) and T(MI) represents an Invar effect. The two phase transitions, which surprisingly mimic the classic freezing transition of water, suggest an exotic ground state driven by an extraordinary coupling between spin, orbit, and lattice degrees of freedom.

Experimental electronic structure of the metallic pyrochlore iridate Bi2Ir2O7.

Angle-resolved photoemission measurements have been performed on Bi2Ir2O7 single crystals, a metallic end-member of the family of pyrochlore iridates. The density of states, the Fermi surface, and the near-Fermi-level band dispersion in the plane perpendicular to the (1, 1, 1) direction were all measured and found to be in rough overall agreement with our LDA + SOC density functional calculations. Assuming that this same calculation approach will extend to other members of the pyrochlore iridates, the overall agreement we found increases the possibility that some of the novel predicted phases such as quantum spin-ice or Weyl Fermion states will exist in this family of compounds.

Strong magnetic instability in correlated metallic Bi2Ir2O7.

We report an experimental/theoretical study of single-crystal Bi(2)Ir(2)O(7) that possesses a metallic state with strongly exchange-enhanced paramagnetism. The ground state of Bi(2)Ir(2)O(7) is characterized by the following features: (1) a divergent low-temperature magnetic susceptibility that indicates no long-range order down to 50 mK; (2) strongly field-dependent coefficients of the low-temperature T and T(3) terms of the specific heat; (3) a conspicuously large Wilson ratio R(W) ≈ 53.5; and (4) unusual temperature and field dependences of the Hall resistivity that abruptly change below 80 K, without any clear correlation with the magnetic behavior. All these unconventional properties suggest the existence of an exotic ground state in Bi(2)Ir(2)O(7).

Correlated giant dielectric peaks and antiferromagnetic transitions near room temperature in pure and alkali-doped BaMnO(3-δ).

We report structural, magnetic, dielectric and thermal properties of single-crystal BaMnO(2.99) and its derivatives BaMn(0.97)Li(0.03)O(3) and Ba(0.97)K(0.03)MnO(3). The hexagonal 15R-BaMnO(2.99) perovskite phase is a known antiferromagnetic insulator that orders at a Néel temperature T(N) = 220 K. We find dilute Li and K doping change the ratio of cubic to hexagonal layers and cause drastic changes in the dielectric and magnetic properties. Unusually large high-temperature magnetoelectric shifts (up to 85%) are observed near temperatures at which pronounced peaks in the dielectric constant are observed for applied electric fields along either the c or a axis, respectively. The temperatures of the dielectric peaks are strongly correlated with anomalies in the c- or a-axis magnetic susceptibility and the specific heat for all compositions studied. All our data suggest that the strongly anisotropic magnetic and dielectric anomalies (which occur near, or above room temperature) originate from the same Mn ion sites, which implies these materials form an exceptional class of magnetoelectrics.