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In the scientific description of unconventional transport properties ofoxides (spin-dependent transport, superconductivity etc.), the spin-statedegree of freedom plays a fundamental role. Because of this, temperature- ormagnetic field-induced spin-state transitions are in the focus of solid-statephysics. Cobaltites, e.g. LaCoO3, are prominent examples showing these spintransitions. However, the microscopic nature of the spontaneous spin crossoverin LaCoO3 is still controversial. Here we report magnetostriction measurementson LaCoO3 in magnetic fields up to 70 T to study the sharp, field-inducedtransition at Hc ~ 60 T. Measurements of both longitudinal and transversalmagnetostriction allow us to separate magnetovolume and magnetodistortivechanges. We find a large increase in volume, but only a very small increase intetragonal distortion at Hc. The results, supported by electronic energycalculations by the configuration interaction cluster method, providecompelling evidence that above Hc LaCoO3 adopts a correlated low spin/high spinstate.

Mechanism of spin crossover in LaCoO3 resolved by shape magnetostriction in pulsed magnetic fields