Transition to Long Range Magnetic Order in the Highly Frustrated Insulating Pyrochlore Antiferromagnet Gd_2Ti_2O_7

Abstract

Experimental evidence from measurements of the a.c. and d.c. susceptibility, and heat capacity data show that the pyrochlore structure oxide, Gd_2Ti_2O_7, exhibits short range order that starts developing at 30K, as well as long range magnetic order at $T\sim 1$K. The Curie-Weiss temperature, $θ_{CW}$ = -9.6K, is largely due to exchange interactions. Deviations from the Curie-Weiss law occur below $\sim$10K while magnetic heat capacity contributions are found at temperatures above 20K. A sharp maximum in the heat capacity at $T_c=0.97$K signals a transition to a long range ordered state, with the magnetic specific accounting for only $\sim$ 50% of the magnetic entropy. The heat capacity above the phase transition can be modeled by assuming that a distribution of random fields acts on the $^8S_{7/2}$ ground state for Gd$^{3+}$. There is no frequency dependence to the a.c. susceptibility in either the short range or long range ordered regimes, hence suggesting the absence of any spin-glassy behavior. Mean field theoretical calculations show that no long range ordered ground state exists for the conditions of nearest-neighbor antiferromagnetic exchange and long range dipolar couplings. At the mean-field level, long range order at various commensurate or incommensurate wave vectors is found only upon inclusion of exchange interactions beyond nearest-neighbor exchange and dipolar coupling. The properties of Gd$_2Ti_2O_7 are compared with other geometrically frustrated antiferromagnets such as the Gd_3Ga_5O_{12} gadolinium gallium garnet, RE_2Ti_2O_7 pyrochlores where RE = Tb, Ho and Tm, and Heisenberg-type pyrochlore such as Y_2Mo_2O_7, Tb_2Mo_2O_7, and spinels such as ZnFe_2O_4