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While nanoalloys are of paramount scientific and practical interests, themain processes leading to their formation are still poorly understood. Keystructural features in the alloy systems, including crystal phase, chemicalordering, and morphology, are challenging to control at the nanoscale, makingit difficult to transfer their usage to industrial applications. In thiscontribution, we focus on the gold/silver system that has two of the mostprevalent noble metals, and combine experiments with simulations to uncover theformation mechanisms at the atomic-level. Nanoparticles are produced usingstate-of-the-art inert-gas aggregation source and analyzed using transmissionelectron microscopy and energy-dispersive x-ray spectroscopy.Machine-learning-assisted molecular dynamics simulations are employed to modelthe crystallization process from liquid droplets to nanocrystals. Our studyfinds a preponderance of nanoparticles with five-fold symmetric morphology,including icosahedron and decahedron which is consistent with previous resultson mono-metallic nanoparticles. However, we observe that gold atoms, ratherthan silver atoms, segregate at the surface of the obtained nanoparticles forall the considered alloy compositions. These segregation tendencies are incontrast to previous studies and have consequences on the crystallizationdynamics and the subsequent crystal ordering. We finally show that theunderpinnings of this surprising segregation dynamics is due to charge transferand electrostatic interactions rather than surface energy considerations.

Exploring the formation of gold/silver nanoalloys with gas-phase synthesis and machine-learning assisted simulations