Experimental measurement of the isolated magnetic susceptibility

The isolated susceptibility $\chi_{\rm I}$ may be defined as a (non-thermodynamic) average over the canonical ensemble, but while it has often been discussed in the literature, it has not been clearly measured. Here, we demonstrate an unambiguous measurement of $\chi_{\rm I}$ at avoided nuclear-electronic level crossings in a dilute spin ice system, containing well-separated holmium ions. We show that $\chi_{\rm I}$ quantifies the superposition of quasi-classical spin states at these points, and is a direct measure of state concurrence and populations.