The compound $\lambda${}-(BETS)2FeCl4 provides an effective demonstration of the interaction of $\pi${} conduction electron and d-electron localized moment systems in molecular crystalline materials where antiferromagnetic insulating and magnetic field induced superconducting states can be realized. The metal-insulator transition has been thought to be cooperative, involving both the itinerant $\pi${}-electron and localized d-electron spins where antiferromagnetic order appears in both systems simultaneously. However, recent specific-heat data has indicated otherwise [H. Akiba, S. Nakano, Y. Nishio, K. Kajita, B. Zhou, A. Kobayashi, and H. Kobayashi, J. Phys. Soc. Jpn. 78, 033601 (2009)]: although the $\pi${}-electron system orders antiferromagnetically and produces a metal-insulator transition, a paramagnetic d-electron state remains. We report F57e M\"ossbauer measurements that support the paramagnetic model provided the d-electron spins remain in a fast relaxation state below the transition. From the measured hyperfine fields, we also determine the temperature dependence of the $\pi${}$-${}d electron exchange field.
18 October 2001 in European Journal of Inorganic Chemistry