Abstract
Abstract Typical molecular-based magnets, decamethylferrocenium tetracyanoethenide ([DMeFc][TCNE]) and decamethylferrocenium tetracyanoquinodimethanide ([DMeFc][TCNQ]), have been studied by means of adiabatic calorimetry. The Curie temperature of [DMeFc][TCNE] was determined to be Tc - 4.74 K. The excess entropy derived from the observed heat-capacity anomaly was very close to the expected magnetic entropy, 2 R In 2. Detailed analysis of the heat-capacity anomaly revealed that [DMeFc][TCNE] is a good one-dimensional (ID) Ising magnet. Two structural phase transitions were found for the first time at 248.7 and 281.8 K, and attributed to the orientational order-disorder character of the TCNE anion. For [DMeFc][TCNQ] an antiferromagnetic phase transition was observed at TN = 2.54 K. The magnetic lattice anisotropy of the TCNQ salt is smaller than that of the TCNE salt.
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