Raman spectra of the delafossite CuGa 1-x Cr x O 2 (0 ≤ x ≤ 1) solid solution films have been measured in the temperature range from 80 to 823 K. Raman phonon modes are observed at 224 (A g ), 328 (A 2u ), 396 (E g ), and 757 (A 1g ) cm −1 for the CuGaO 2 film, and phonon modes of the CuCrO 2 film are around 211 (A g ), 324 (A 2u ), 458 (E g ), and 712 (A 1g ) cm −1 , respectively. The A 1g phonon mode has a distinct redshift with increasing Cr composition, which indicates that the interatomic potential becomes weaker between Cu and O atoms. Except Raman modes at the Brillouin zone center, the additional phonon modes in the spectral range of 500−670 cm −1 were observed due to Raman selection rules being relaxed by the crystal defects. With increasing temperature, the A 1g phonon mode undergoes a larger phonon softening but a smaller line broadening relative to that of the E g phonon mode, which indicated the anisotropic behavior for the delafossite CuGa 1-x Cr x O 2 films. The nonlinear temperature dependence of the phonon frequency and linewidth is an indication of nonharmonic lattice dynamics. The Raman shift and the linewidth of the E g and A 1g optical modes as a function of temperature were studied as an experimental evidence of the combined effect of lattice expansion and anharmonic phonon-phonon interaction. And the three-phonon anharmonic coupling plays the dominant role in the anharmonicity behavior. The phonon anharmonicity behavior of the CuGaO 2 and CuCrO 2 films is slightly different. The larger Γ 0 is intrinsic for the A 1g mode of the CuGa 0.8 Cr 0.2 O 2 film due to the broadening by the crystalline defects, which perturb the translation symmetry of the harmonic crystal, making the momentum conservation rule for phonon scattering partially relaxed.
K E Y W O R D Sdelafossite, phonon mode, Raman spectra, temperature, vibrational anharmonicity