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Three high-spin phases recently discovered in the spin-crossover systemMn(taa) are identified through analysis by a combination of first-principlescalculations and Monte Carlo simulation as a low-temperature Jahn-Tellerordered (solid) phase, an intermediate-temperature dynamically correlated(liquid) phase, and an uncorrelated (gas) phase. In particular, the Jahn-Tellerliquid phase arises from competition between mixing with low-spin impurities,which drive the disorder, and inter-molecular strain interactions. The latterare a key factor in both the spin-crossover phase transition and themagnetoelectric coupling. Jahn-Teller liquids may exist in other spin-crossovermaterials and materials that have multiple equivalent Jahn-Teller axes.

Three Jahn-Teller states of matter in the spin-crossover system Mn(taa)