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A few organic conductors show a diversity of exciting properties like Mottinsulating behaviour, spin liquid, antiferromagnetism, bad metal orunconventional superconductivity controlled by small changes in temperature,pressure or chemical substitution. While such a behaviour can betechnologically relevant for functional switches, a full understanding of itsmicroscopic origin is still lacking and poses a challenge in condensed matterphysics since these phases may be a manifestation of electronic correlation.Here we determine from first principles the microscopic nature of theelectronic phases in the family of organic systemskappa-(ET)2Cu[N(CN)2]BrxCl1-x by a combination of density functional theorycalculations and the dynamical mean field theory approach in a new form adaptedfor organic systems. By computing spectral and optical properties we are ableto disentangle the origin of the various optical transitions in these materialsand prove that correlations are responsible for relevant features. Remarkably,while some transitions are inherently affected by correlations, others arecompletely uncorrelated. We discuss the consequences of our findings for thephase diagram in these materials.

Unveiling the microscopic nature of correlated organic conductors: the case of kappa-(BEDT-TTF)2Cu[N(CN)2]BrxCl1-x