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In this article we study the effects of a partial substitution of Ba with thesmaller cation Ca in the layered cobaltites YBaCo_2O_{5+\delta} for \delta\approx 0.5. Neutron thermodiffractograms are reported for the compoundsYBa_{0.95}Ca_{0.05}Co_2O_{5.5} (x_{Ca}=0.05) and YBa_{0.90}Ca_{0.10}Co_2O_{5.5}(x_{Ca}=0.10) in the temperature range 20 K \leq T \leq 300 K, as well as highresolution neutron diffraction experiments at selected temperatures for thesamples x_{Ca}=0.05, x_{Ca}=0.10 and the parent compound x_{Ca}=0. We havefound the magnetic properties to be strongly affected by the cationicsubstitution. Although the "122" perovskite structure seems unaffected by Caaddition, the magnetic arrangements of Co ions are drastically modified: theantiferromagnetic (AFM) long-range order is destroyed, and a ferrimagneticphase with spin state order is stabilized below T \sim 290 K. For the samplewith x_{Ca}=0.05 a fraction of AFM phase coexists with the ferrimagnetic onebelow T \sim 190 K, whereas for x_{Ca}=0.10 the AFM order is completely lost.The systematic refinement of the whole series has allowed for a betterunderstanding of the observed low-temperature diffraction patterns of theparent compound, YBaCo_2O_{5.5}, which had not yet been clarified. A two-phasescenario is proposed for the x_{Ca}=0 compound which is compatible with thephase coexistence observed in the x_{Ca}=0.05 sample.

physical review. b, condensed matter and materials physics

Probing phase coexistence and stabilization of the spin-ordered  ferrimagnetic state by Calcium addition in the YBa_{1-x}Ca_{x}Co_{2}O_{5.5}  layered cobaltites using neutron diffraction