Many technological applications exploit a variety of magnetic
structures, or magnetic phases, to produce and optimise solid-state
functionality. However, most research advances are restricted to a
reduced number of phases owing to computational and resource
constraints. This thesis presents an ab-initio theory to
efficiently describe complex magnetic phases and their
temperature-dependent properties. The central assumption is that
magnetic phases evolve slowly compared with the underlying
electronic structure from which they emerge. By describing how the
electronic structure adapts to the type and extent of magnetic
order, a theory able to describe multi-spin correlations and their
effect on the magnetism at finite temperature is obtained. It is
shown that multi-spin correlations are behind the temperature and
magnetic field dependence of the diverse magnetism in the heavy
rare earth elements. Magnetically frustrated Mn-based materials and
the effect of strain are also investigated. These studies
demonstrate that the performance of solid-state refrigeration can
be enhanced by multi-spin effects.
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