Infrared reflection measurements of the half-filled two-dimensional organic conductors κ-(BEDT-TTF)2Cu[N(CN)2]BrxCl1−x were performed as a function of temperature (5 K < T < 300 K) and Br-substitution (x = 0%, 40%, 73%, 85%, and 90%) in order to study the metal-insulator transition. We can distinguish absorption processes due to itinerant and localized charge carriers. The broad mid-infrared absorption has two contributions: transitions between the two Hubbard bands and intradimer excitations from the charges localized on the (BEDT-TTF)2 dimer. Since the latter couple to intramolecular vibrations of BEDT-TTF, the analysis of both electronic and vibrational features provides a tool to disentangle these contributions and to follow their temperature and electronic-correlations dependence. Calculations based on the cluster model support our interpretation.

The polarized optical conductivity data of two ~-phase charge-transfer salts of b~s-(ethylenedithio)-tetrathiafulvalene: ~-(BEDT-TTF)2(Hg(SCN)2Br] and ~-(BEDT-TTF)2 [Hg(SCN)C12), are, discussed.

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