A series of 2, 2′: 6′, 2′′-terpyridine-based chromophores (L1, L2, L3 and L4) with intramolecular 'push–pull'structure have been designed and synthesized. The single crystals of L1, L2 and L4 were obtained and solved by X-ray diffraction analysis. The photophysical behavior and the connections between structure and properties of the chromophores were investigated both experimentally and theoretically. It is revealed that the chromophores ...