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We investigated the electronic structure and lattice dynamics of double perovskite NdBaMn 2 O 6  single crystals through spectroscopic ellipsometry and Raman scattering spectroscopy. The optical absorption band centered at approximately 0.88 eV was assigned to on-site  d – d  transitions in Mn, whereas the optical feature at approximately 4.10 eV was assigned to charge-transfer transitions between the 2 p  state of O and 3 d  state of Mn. Analysis of the temperature dependence of the  d-d  transition indicated anomalies at 290 and 235 K. The activated phonon mode, which appeared at approximately 440 cm −1  alongside with the enhancement of the 270 cm −1  phonon mode, coupled strongly to the metal–insulator transition at 290 K, which was associated with a charge/orbital ordering. Moreover, the MnO 6  octahedral breathing mode at 610 cm −1  exhibited softening at a temperature lower than 235 K (temperature of the antiferromagnetic phase transition), which revealed the strong coupling between the lattice and magnetic degrees of freedom. The spin–phonon coupling constant obtained was  λ  = 2.5 cm −1 . These findings highlight the importance of charge–orbital–spin interactions in establishing NdBaMn 2 O 6  phases with novel properties.

Optical Study of the Electronic Structure and Lattice Dynamics of NdBaMn2O6 Single Crystals