Ruthenium(II) Photosensitizers of Tridentate Click-Derived Cyclometalating Ligands: A Joint Experimental and Computational Study

A systematic series of heteroleptic bis(tridentate)ruthenium(II) complexes of click-derived 1,3-bis(1,2,3-triazol-4-yl)benzene N boolean AND C boolean AND N-coordinating ligands was synthesized, analyzed by single crystal X-ray diffraction, investigated photophysically and electrochemically, and studied by computational methods. The presented comprehensive characterization allows a more detailed understanding of the radiationless deactivation mechanisms. Furthermore, we provide a fully optimized synthesis and systematic variations towards redox-matched, broadly and intensely absorbing, cyclometalated ruthenium(II) complexes. Most of them show a weak room-temperature emission and a prolonged excited-state lifetime. They display a broad absorption up to 700 nm and high molar extinction coefficients up to 20?000?M-1?cm-1 of the metal-to-ligand charge transfer bands, resulting in a black color. Thus, the complexes reveal great potential for dye-sensitized solar-cell applications.