Anion polarity-induced self-doping in a purely organic paramagnetic conductor, α′-α′-(BEDT-TTF) 2 (PO-CONH- m -C 6 H 4 SO 3 )·H 2 O where BEDT-TTF is bis(ethylenedithio)tetrathiafulvalene and PO is the radical 2,2,5,5-Tetramethyl-3-pyrrolin-1-oxyl

Abstract A new BEDT-TTF-based salt with an organic free radical, α′-α′-(BEDT-TTF) 2 (PO-CONH- m -C 6 H 4 SO 3 )·H 2 O, has been prepared. The crystal structure consists of alternating donor and anion/water layers propagated along the c axis. The anisotropic radical anions form a head-to-head arrangement, which provides a permanent dipole moment. The effect on the nearest donor layer has been estimated to be 4.0 V. The salt has two crystallographically independent donor layers (A and B), one of which (A) is surrounded by the negative ends of the anion layer dipole whereas the B layers are bordered by the positive ends of the dipole. This structural feature suggests that layers A and B have different Fermi levels. To eliminate the imbalance, self-doping occurs whereby electron density is transferred from layer A to B. The temperature dependence of the magnetic susceptibility has 11.1% of extra Curie spins, from which a doping ratio of 12.7% has been estimated.