Cooperativity of dynamics of 18-crown-6 molecule forming one-dimensional chain in Cs2(18-crown-6)3[Ni(dmit)2]2.

Heat capacity of Cs2(18-crown-6)3[Ni(dmit)2]2 was measured by adiabatic calorimetry. A broad thermal anomaly was observed around 225 K. The entropy gain (about 52 J K(-1) mol(-1)) is much larger than that expected for twofold disordering of 18-crown-6 assumed in the previous structure analysis. The shape of thermal anomaly was qualitatively explained by a linear Ising model developed for cooperative disordering in polymers. The 18-crown-6 molecules forming a one-dimensional chain in the crystal are orientationally disordered with moderate cooperativity.