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Phase-formation of surface alloying by spinodal decomposition has beenstudied for the first time at an electrified interface. For this aim Zn waselectrodeposited on Au(111) from the ionic liquid AlCl3-MBIC (58:42) containing1 mM Zn(II) at different potentials in the underpotential range correspondingto submonolayer up to monolayer coverage. Structure evolution was observed byin situ electrochemical scanning tunneling microscopy (STM) at different timesafter starting the deposition via potential jumps and at temperatures of 298 Kand 323 K. Spinodal or labyrinth two-dimensional structures predominate atmiddle coverage, both in deposition and dissolution experiments. They arecharacterized by a length scale of typically 5 nm which has been determinedfrom the power spectral density of the STM images. Structure formation andsurface alloying is governed by slow kinetics with a rate constant k withactivation energy of 120 meV and preexponential factor of 0.17 Hz. Theevolution of the structural features is described by a continuum model and isfound to be in good agreement with the STM observations. From the experimentaland model calculation results we conclude that the two-dimensionalphase-formation in the Zn on Au(111) system is dominated by surface alloying.The phase separation of a Zn-rich and a Zn-Au alloy phase is governed by 2Dspinodal decomposition.

Two-dimensional connective nanostructures of electrodeposited Zn on Au(111) induced by spinodal decomposition