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We report the influence of Ni/Mn ordering on the spin-phonon coupling inmultifunctional La2NiMnO6. Three types of films with different levels ofstructural order, including long-range Ni/Mn cation order, cation disorder, andan admixture of the ordered and disordered phases, are compared by polarizedmicro-Raman spectroscopy and magnetometry. Each film displays a strongdependence on the polarization configuration and a unique set of Raman activephonon excitations. Long-range cation ordering results in the splitting ofRaman active phonon peaks because of Brillouin zone folding and loweringsymmetry. Phonon mode softening begins clearly at a distinct temperature foreach sample revealing a strong spin-lattice interaction. It follows closely themagnetization curve in ordered films. Unlike the admixture and the orderedfilms, softening behavior is strongly suppressed in the cation-disorderedfilms. These differences may be understood based on the variation in amplitudeof the spin-spin correlation functions due to the local Ni/Mn cation ordering.

Influence of Ni/Mn cation order on the spin-phonon coupling in multifunctional La2NiMnO6 epitaxial films by polarized Raman spectroscopy