Emergent Electrochemistry in Spin Ice: Debye-H\"{u}ckel Theory and Beyond

Understand

The low-temperature picture of dipolar spin ice in terms of the Coulomb fluid of its fractionalised magnetic monopole excitations has allowed analytic and conceptual progress far beyond its original microscopic spin description.

• Here we develop its thermodynamic treatment as a `magnetolyte', a fluid of singly and doubly charged monopoles, an analogue of the electrochemical system ${\rm 2 H_2O = H_3O^+ +OH^- = H_4O^{2+} + O^{2-}}$, but with perfect symmetry between oppositely charged ions.
• For this lattice magnetolyte, we present an analysis based on Debye-H\"uckel theory, which is accurate at all temperatures and incorporates `Dirac strings' imposed by the microscopic ice rule constraints at the level of Pauling's approximation.
• Our results are in close agreement with the specific heat from numerical simulations as well as new experimental measurements with an improved lattice correction, which we present here, on the spin ice materials $\mathrm{Ho_2Ti_2O_7}$ and $\mathrm{Dy_2Ti_2O_7}$.