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Despite the great technological and scientific importance, a well-controlledcoupled behavior in magnetoelectric multiferroic materials at room temperatureremains challenging. We demonstrate that the self-ordered A2BBO6 (e.g., A = La,B = Mn, and B = Ni) double perovskites provide a unique alternative opportunityto control and/or to induce such behavior in oxides. In this paper, we outlineand discuss the various challenges and bottleneck issues related to this classof materials using La2NiMnO6 as a prototype. Details of the synthesisstrategies, using pulsed laser deposition as a central tool, to obtain ameticulous control over cation ordering is illustrated. The possible impact ofNi/Mn cation ordering on the magnetic ground states, ferromagnetic transitiontemperature, phonon behavior, and spin-phonon coupling are presented. Ourresults are also compared with the current literature on related compounds.

Multiferroic double perovskites: Opportunities, Issues and Challenges