Spin glass like behavior in the novel layered material Na_2IrO_3

Abstract

We have synthesized the novel material Na_2IrO_3 and studied its structure, transport, magnetic, and thermal properties using powder x-ray diffraction (PXRD), electrical resistivity, isothermal magnetization M versus magnetic field H, static \chi and dynamic \chi_ac magnetic susceptibility versus temperature T, and heat capacity C versus T measurements. Na_2IrO_3 crystallizes in the monoclinic C2/c (No. 15) structure which is made up of Na and NaIr_2O_6 layers alternately stacked along the c axis. From a Rietveld refinement of the PXRD pattern we identify atomic disorder arising from a mixing of Ir and Na sites within the NaIr_2O_6 layers. The \chi data in H = 1 T shows Curie-Weiss behavior at high T > 100 K with an effective moment \mu_eff = 1.82(1) \mu_B indicating an effective spin S_eff = 1/2 on the Ir^{4+} moments. A Weiss temperature \theta = - 62(1) K indicates substantial antiferromagnetic interactions between these S_eff = 1/2, Ir^{4+} moments. The \chi data in low field show a sharp cusp at T_g = 5.5 K and there is a bifurcation between zero-field-cooled (ZFC) and field-cooled (FC) data below this T. The \chi_ac data also show a sharp cusp at T_g = 5.5 K at a frequency f = 1 Hz which moves to higher temperatures with increasing f. We did not observe any anomaly at T_g in our C measurements and only a broad shoulder was observed at a much higher T = 12 K. Our results indicate that in Na_2IrO_3, a spin-glass like state occurs below the freezing temperature T_g = 5.5 K and this freezing most likely arises either from structural disorder or geometrical magnetic frustration.