The effect of Eu3+ion doping in the La sites of single-crystal La4/3Sr5/3Mn2O7was investigated. Electron spin resonance(ESR) was applied to La4/3Sr5/3Mn2O7and(La0.8Eu0.2)4/3Sr5/3Mn2O7single crystals. A phase separation and phase transitions were observed from the ESR spectra data. Between 350 K and 300 K, both paramagnetic resonance(PMR)and anisotropic ferromagnetic resonance(FMR) lines were observed in the ab plane and the c axis direction, suggesting a coexistence of the paramagnetic(PM) phase and the ferromagnetic(FM) phase. The magnetization measurement reveals a spin-glass-like behavior in single-crystal(La0.8Eu0.2)4/3Sr5/3Mn2O7below the temperature of spin freezing Tf(～ 29.5 K).
