Single-ion properties of the S eff = 1 2 XY antiferromagnetic pyrochlores Na A ' Co 2 F 7 ( A ' = Ca 2 + , Sr 2 + )
The antiferromagnetic pyrochlore material NaCaCo 2 F 7 is a thermal spin liquid over a broad temperature range (≈140 K down to T F =2.4 K), in which magnetic correlations between Co 2+ dipole moments explore a continuous manifold of antiferromagnetic XY states. The thermal spin liquid is interrupted by spin freezing at a temperature that is ~2% of the mean-field interaction strength, leading to short-range static XY clusters with distinctive relaxation dynamics. Here we report the low-energy inelastic neutron scattering response from the related compound NaSrCo 2 F 7 , confirming that it hosts the same static and dynamic spin correlations as NaCaCo 2 F 7 . We then present the single-ion levels of Co 2+ in these materials as measured by inelastic neutron scattering. An intermediate spin-orbit coupling model applied to an ensemble of trigonally distorted octahedral crystal fields accounts for the observed transitions. The single-ion ground state of Co 2+ is a Kramers doublet with a strongly XY-like g tensor ( gxy/gz ~3). The local disorder inherent from the mixed pyrochlore A sites (Na + /Ca 2+ and Na + /Sr 2+ ) is evident in these measurements as exaggerated broadening of some of the levels. A simple model that reproduces the salient features of the single-ion spectrum produces approximately 8.4% and 4.1% variation in the z and xy components of the g tensor, respectively. In conclusion, this study confirms that an S eff = 1/2 model with XY antiferromagnetic exchange and weak exchange disorder serves as a basic starting point in understanding the low-temperature magnetic behavior of these strongly frustrated magnets.