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Magnetic and Thermal Properties of Crystals Including Isolated Clusters. II. Heat Capacity of Co3(C5H5)3S2 from 15 to 270 K and Mechanism of Phase Transition

Heat capacity of Co3(C5H5)3S2 was measured between 15 and 270 K. A phase transition was discovered at 192.5±0.1 K with the transition enthalpy and the entropy of 5253.4 J mol−1 and 28.894 J K−1 mol−1, respectively. The transition entropy is well described as the sum of the configurational entropy of Rln8 due to cyclopentadienyl rings and the magnetic contribution of Rln4. The transition behavior is satisfactorily accounted for in the whole temperature region investigated in terms of the cooperative coupling between the orientational motion of the rings and the electronic states of a molecule on the basis of the Chesnut exciton model modified by the present authors. The model proposed here is to take both the temperature dependences of the energy parameters and the inversion of the spin state at higher temperatures into account. The measurements of infrared spectra and proton magnetic resonance were made as a function of temperature. These results are favorable to the present model. The electron spin reson...