High-pressure crystal growth and magnetic and electrical properties of the quasi-one dimensional osmium oxide Na2OsO4

Na2OsO4 crystals were grown by a NaCl flux method under high pressure. It crystallizes in the Ca2IrO4-type structure without having additional elements or metal vacancies, which are usually accommodated. It appears that Na2OsO4 is a metal-stoichiometric Ca2IrO4-type compound never been synthesized to date. Na2OsO4 has the octahedral environment of Os6+O6 so that the electronic configuration is 5d2, suggesting the magnetic S=1 ground state. However, magnetization, electrical resistivity, and specific heat measurements indicated that the non-magnetic S=0 state is much likely for Na2OsO4 than the S=1 state. Band structure calculations and the structure analysis found that the disagreement is probably due to the statically uniaxial compression of the OsO6 octahedra, resulting in splitting of the t 2 g band.