Transition metal dichalcogenides (TMDs) semiconductors with direct bandgap are suitable for use in optoelectronic devices such as LEDs and solar cells. Optimized optically active centers (functional units derived from few-layers of 2D [in]organic heterostructures), able to convert incoming photons into free electrons, can be thought as embedded into an active conductive matrix which drives the generated photoelectrons towards an external circuit. Using advanced Molecular Dynamics, (TD)DFT, and Green's function-based techniques, bandgap tunability will be investigated, in order to ultimately design novel TMD-based sollar cells.