Surface-bound heteroleptic copper(I) dyes [Cu(L anchor )(L ancillary )] + are assembled using the "surfaces-as-ligands, surfaces as complexes" (SALSAC) approach by three different procedures. The anchoring and ancillary ligands chosen are ((6,6 -dimethyl-[2,2 -bipyridine]-4,4 -diyl)-bis(4,1-phenylene))bis(phosphonic acid) (3) and 4,4 -bis(4-iodophenyl)-6,6 -diphenyl-2,2 -bipyridine (4), respectively. In the first SALSAC procedure, the FTO/TiO 2 electrode is functionalized with 3 in the first dye bath, and then undergoes ligand exchange with the homoleptic complex [Cu (4)