Antiferromagnetic Mott insulating state in single crystals of the hexagonal lattice material Na2IrO3

Abstract: We have synthesized single crystals of Na_2IrO_3 and studied their structure, transport, magnetic, and thermal properties using powder x-ray diffraction (PXRD), electrical resistivity, isothermal magnetization M versus magnetic field H, magnetic susceptibility \chi versus temperature T, and heat capacity C versus T measurements. Na_2IrO_3 crystallizes in the monoclinic \emph{C2/c} (No. 15) type structure which is made up of Na and NaIr_2O_6 layers alternately stacked along the c axis. The \chi(T) data show Curie-Weiss behavior at high T > 200K 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 large Weiss temperature \theta = - 116(3)K indicates substantial antiferromagnetic interactions between these S_eff = 1/2, Ir^4+ moments. Sharp anomalies in \chi(T) and C(T) data indicate that Na_2IrO_3 undergoes a transition into a long-range antiferromagnetically ordered state below T_N = 15 K. The magnetic entropy at T_N is only about 20% of what is expected for S_eff = 1/2 moment ordering. The reduced entropy and the small ratio T_N/\theta \approx 0.13 suggest geometrical magnetic frustration and/or low-dimensional magnetic interactions in Na_2IrO_3. In plane resistivity measurements show insulating behavior. This together with the local moment magnetism indicates that bulk Na_2IrO_3 is a Mott insulator.