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The preparation of cation-ordered thin films of correlated oxides is of great interest for both fundamental and applied research. The scientific long-term vision is strongly motivated by the perspective of studying electronic correlations in condensed matter without the presence of chemical or quenched disorder. A promising material platform provides double perovskite A2BB’O6 bulk samples with different types of B/B’ ordering. However, the growth of A- and/or B-site-ordered correlated oxide thin films is known to be a challenging task. In this review, we evaluate the growth of double perovskite A2BB’O6 thin films by means of well-elaborated physical vacuum deposition techniques, such as pulsed laser deposition (PLD) and sputtering and compare them with a close-to-equilibrium growth with the metalorganic aerosol deposition (MAD) technique. The latter was further developed to grow an emergent interfacial double perovskite phase in LaNiO3/LaMnO3 superlattices, and finally, by way of a layer-by-layer route. The growth of La2CoMnO6 films on SrTiO3(111) substrates by sequential deposition of single perovskite layers of LaCoO3/LaMnO3/LaCoO3/… was demonstrated and the film properties were compared to those obtained within the state-of-the art growth mode.

We report magneto-dielectric properties of partially B-site ordered monoclinic Tb2CoMnO6 double perovskite thin film epitaxially grown by metalorganic aerosol deposition technique.Transmission electron microscopy and electron energy loss spectroscopy mapping shows the presence and distribution of both Co 2+ and Co 3+ ions in the film, evidencing a partial B-site disorder, which was further confirmed by the observation of reduced saturation magnetization at low temperatures. The ferromagnetic Curie temperature, TC=110 K, is slightly higher as compared to the bulk value (100 K) probably due to an in plane tensile strain. Remarkably, a short range ordering of spins at T*~190 K>>TC was established and assigned to the B-site disorder in the film.Two different dielectric relaxation peaks have been observed; they merge at the same temperature T* of short range spin correlations. Moreover, an unexpected high temperature dipolar relaxorglass-like transition at T~T* was observed, at which a coupling to short range magnetic correlations results in a 4% magneto-dielectric coupling.

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Two series of B-site ordered, double-perovskite A2CoMnO6 and A2NiMnO6 (A = La, Pr, Nd, Sm, Gd) epitaxial films with thickness d ~ 100 nm were grown on SrTiO3(111) substrates via metalorganic aerosol deposition. Polarization and temperature-dependent Raman spectroscopy were carried out in order to determine the spin-phonon coupling constant, λ, and the impact of the A-site cation radius on the phonon properties. The reduction of the A-site cation radius from La3+ down to Gd3+ systematically shifts the Raman modes to lower wavenumbers, and decreases the magnetization-induced softening of the Ag breathing mode, described by the spin-phonon coupling constant, λ, which changes from λ = 1.42 cm−1 (La2CoMnO6) and λ = 1.53 cm−1 (La2NiMnO6) down to λ = 0.58 cm−1 (Gd2CoMnO6) and λ = 0.44 cm−1 (Gd2NiMnO6). A similar effect of the A-cation radius was established for the c-lattice parameter and Curie temperature, TC, in this series of double-perovskite films. Our observations directly demonstrate a strong impact of the lattice structure on the ferromagnetic superexchange interaction in double perovskites. Moreover, the A2CoMnO6 and A2NiMnO6 series exhibit very similar behavior of spin-phonon coupling due to the only moderate difference of Co2+ and Ni2+ cation size.