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The compound lambda-(BETS)2FeCl4 provides an effective demonstration of theinteraction of pi-conduction electron and d-electron localized moment systemsin molecular crystalline materials where antiferromagnetic insulating andmagnetic field induced superconducting states can be realized. Themetal-insulator transition has been thought to be cooperative, involving boththe itinerant pi- electron and localized d-electron spins whereantiferromagnetic order appears in both systems simultaneously. However, recentspecific heat data has indicated otherwise [Akiba et al., J. Phys. Soc. Japan78,033601(2009)]: although the pi-electron system orders antiferromagneticallyand produces a metal-insulator transition, a "mysterious" paramagneticd-electron state remains. We report 57Fe Mossbauer measurements that supportthe paramagnetic model, provided the d-electron spins remain in a fastrelaxation state below the transition. From the measured hyperfine fields, wealso determine the temperature dependence of the pi-d electron exchange field.

Mossbauer spectroscopy study of the "mysterious" magnetic transition in lambda-(BETS)2FeCl4