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The intense coupling by gradient doping offers an effective approach to enable the plasmon resonances of Ti excited by visible light. The Ti-based plasmonic heterostructure potentially opens an alternative avenue towards sustainable plasmon-enhanced catalysis.Structural, magnetic and theoretical studies of three octahedral mononuclear DyIII complexes with triphenylphosphine oxide and halide ligands are reported. The Cl- and Br- analogues exhibit SMM behavior with energy barriers of 49.1 K and 70.9 K, respectively under a small dc field.