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Non-equilibrium synthesis methods allow to alloy bulk-immiscible elementsinto multinary nanoparticles, which broadens the design space for newmaterials. Whereas sputtering onto solid substrates can combine immiscibleelements into thin film solid solutions, this is not clear for sputtering ofnanoparticles in ionic liquids. Thus, the suitability of sputtering in ionicliquids for producing nanoparticles of immiscible elements is investigated byco-sputtering the systems Au-Cu (miscible), Au-Ru and Cu-Ru (both immiscible),and Au-Cu-Ru on the surface of the ionic liquid 1-butyl-3-methylimidazoliumbis-trifluoromethylsulfonyl)imide [Bmim][(Tf)2N]. The sputtered nanoparticleswere analyzed to obtain (i) knowledge concerning the general formation processof nanoparticles when sputtering onto ionic liquid surfaces and (ii)information, if alloy nanoparticles of immiscible elements can be synthesizedas well as (iii) evidence if the Hume-Rothery rules for solid solubility arevalid for sputtered nanoparticles. Accompanying atomistic simulations usingdensity-functional theory for clusters of different size and ordering confirmthat the miscibility of Au-Cu and the immiscibility of Au-Ru and Cu-Ru governthe thermodynamic stability of the nanoparticles. Based on the matchingexperimental and theoretical results for the NP/IL-systems concerning NPstability, a formation model of multinary NPs in ILs was developed.

Elemental (im-)miscibility determines phase formation of multinary nanoparticles co-sputtered in ionic liquids