Bandwidth-controlled Mott transition in $\kappa -(BEDT-TTF{)}_{2}Cu[N(CN{)}_2]B{r}_{x}C{l}_{1-x}$ I. Optical studies of localized charge excitations

Infrared reflection measurements of the half-filled two-dimensional organic conductors $\kappa$-(BEDT-TTF)${}_2$Cu[N(CN)${}_2$]Br${}_x$Cl${}_{1-x}$ were performed as a function of temperature ($5\mathrm{K}<T<300$ 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.