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Six new complexes of the ligand HQ cy (-4-(cyclohexanecarbonyl)-5-methyl-2-phenyl-2,4-dihydro-3H-pyrazol-3-one) and Ln 3+ ions with emission in the near-infrared (Nd 3+ ) or visible and near-infrared (Sm 3+ , Pr 3+ ) spectral regions were synthesized and characterized using various methods, including single crystal X-ray diffraction. The study demonstrated that both tris complexes [LnQ cy 3 (H 2 O)(EtOH)] and tetrakis-acids [H 3 O][LnQ cy 4 ] can be synthesized by varying the synthetic conditions. The photochemical properties of the complexes were investigated experimentally and theoretically using various molecular spectroscopy techniques and Judd-Ofelt theory. The objective was to quantitatively and qualitatively disclose the influence of complex stoichiometry on its luminescence properties. The study showed that the addition of an extra ligand molecule (in the tetrakis species) increased molar extinction by up to 2 times, affected the shape of photoluminescence spectra, especially of the Pr 3+ complex, and increased the quantum yield of the Sm 3+ complex by up to 2 times. The results obtained from this study provide insights into the luminescent properties of lanthanide coordination compounds, which are crucial for the design and development of novel photonic materials with tailored photophysical properties.