Abstract
It is shown by electron paramagnetic resonance (EPR) and superconductingquantum interference device (SQUID) magnetometry that two spinsystems coexist in conducting layers of the quasi-2D organic metal(BEDO-TTF)2ReO4·H2O: delocalized moments of charge carriers (holes),Iepr(300 K) = 1.62 × 10−4 emu mol−1, and localizedmoments on BEDO-TTF+1, χp(300 K) = 4.25 × 10−4 emu mol−1. The phasetransition Me–Me′ at Tc = 203 K is detected in paramagnetic relaxation, EPR amplitude and resistivity. Magnetic susceptibilities,Iepr and χp, are not sensitive to the transition. Due to fine rearrangement ofReO4 linkedby H2O, the electronic spectrum becomes inhomogeneous. Below the transition exchange-coupledlocalized states within the metallic phase are observed. On cooling, the concentration ofdelocalized moments gradually decreases, contributing to a localized spin system. Thephenomenon is interpreted in terms of short-range antiferromagnetic (AFM) interactionsvia conducting electrons. Below 14 K the AFM coupled states decay, and paramagnetism oflocal moments is recovered.
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