Spin-Glass Transition and Giant Paramagnetism in Heavily Hole-Doped Bi2Sr2Co2Oy

Abstract

Hole-doped single crystals of misfit-layered cobaltate Bi2-xPbxSr2-zCo2Oy (x = 0-0.61, y = 8.28-8.62, and z = 0.01-0.22) have been successfully grown using the optical floating-zone method. Heavier hole doping has been achieved through both Pb substitution in the Bi site and the more effective Sr vacancy formation. The Co4+ : Co3+ ratio can be raised significantly from its original similar to 1 : 1 to 4.5 : 1, as confirmed by iodometric titration. A spin-glass transition temperature of T-g similar to 70K is confirmed by ac susceptibility measurement when the Co4+ : Co3+ ratio becomes higher than 2 : 1, presumably owing to the significantly increased probability of triangular geometrical frustration among antiferromagnetically coupled localized Co4+ spins.