Abstract
Na 2OsO 4 crystals were grown by a NaCl flux method under high pressure. It crystallizes in the Ca 2IrO 4-type structure without having additional elements or metal vacancies, which are usually accommodated. It appears that Na 2OsO 4 is a metal-stoichiometric Ca 2IrO 4-type compound never been synthesized to date. Na 2OsO 4 has the octahedral environment of Os 6+O 6 so that the electronic configuration is 5 d 2, 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 Na 2OsO 4 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 OsO 6 octahedra, resulting in splitting of the t 2 g band.
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