Two new transition
metal oxides with the nominal chemical compositions
of Li4NiOsO6 and Li3Ni2OsO6 were successfully synthesized. Both compounds crystallize
in an ordered rock salt structure type in the monoclinic C2/m space group. The crystal structures were determined
using both synchrotron X-ray and time-of-flight neutron, powder diffraction
data. In both phases, Ni2+ ions are present while oxidation
states of osmium are +6 and +5 in Li4NiOsO6 and
Li3Ni2OsO6, respectively. Ni2+ ions in the hypothetical fully ordered phase form a honeycomb
arrangement in the ab crystallographic plane and
these hexagons are centered by osmium ions. The magnetic layers are
separated along the c axis by the octahedra, which
are centered by Li+ (or Li+/Ni2+,
depending on the chemical compositions). Crystal structure refinements
reveal that there is some degree of mixed occupancy in cationic positions.
Temperature dependent magnetic susceptibility data for both phases
show ferrimagnetic transitions with predominant antiferromagnetic
(AFM) interactions among 3d electrons of nickel and 5d electrons of
osmium. Iso-thermal magnetization loops as a function of the applied
magnetic field below the transition temperatures confirm the ferrimagnetic
nature in magnetic transitions. Temperature dependent heat capacity
data, however, did not exhibit any anomaly in either phase, indicating
the absence of long-range magnetic ordering. The lack of long-range
order for both Os5+ and Os6+-based compounds
was also confirmed by low temperature neutron diffraction data down
to 10 K. Temperature dependent AC magnetic susceptibility data in
various frequencies for both samples indicate that Li4NiOsO6 exhibits spin-glass-like behavior, while the transition temperature
for Li3Ni2OsO6 is nearly frequency
independent.