Abstract

Employing Raman spectroscopy, we have studied the electronic structure of the charge-ordering system, θ-(ET)2X, the dihedral angle (ϕ) of which ranges from 100° to 121°. The most stable metal, θ-(ET)2I3, (ϕ=100°) has a uniform charge distribution in a whole temperature range. The compounds with ϕ>111° have an inhomogeneous charge distribution even above the CO transition, which implies that the charges have localized nature in a whole temperature range. These localized charges are long-range ordered in the CO phase, whereas they are fluctuating randomly or forming short-range ordered domains above the CO phase transition.

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