Magnetic interactions and spin dynamics in the bond-disordered pyrochlore fluoride NaCaCo2 F7

Abstract

© 2019 American Physical Society. We report high-frequency/high-field electron spin resonance (ESR) and high-field magnetization studies on single crystals of the bond-disordered pyrochlore NaCaCo2F7. Frequency- and temperature-dependent ESR investigations above the freezing temperature Tf∼2.4 K reveal the coexistence of two distinct magnetic phases. A cooperative paramagnetic phase, evidenced by a gapless excitation mode, is found along with a spin-glass phase developing below 20 K which is associated with a gapped low-energy excitation. Effective g factors close to 2 are obtained for both modes, in line with pulsed high-field magnetization measurements which show an unsaturated isotropic behavior up to 58 T at 2 K. In order to describe the field-dependent magnetization in high magnetic fields, we propose an empirical model accounting for highly anisotropic ionic g tensors expected for this material and taking into account the strongly competing interactions between the spins which lead to a frustrated ground state. As a detailed quantitative relation between effective g factors as determined from ESR and the local g tensors obtained by neutron scattering [Ross, Phys. Rev. B 93, 014433 (2016)2469-995010.1103/PhysRevB.93.014433] is still sought after, our work motivates further theoretical investigations of the low-energy excitations in bond-disordered pyrochlores.