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Fast-freezing kinetics inside a droplet impacting on a cold surface

Freezing or solidification of impacting droplets is omnipresent in nature and technology, be it a rain droplet falling on a supercooled surface, be it in inkjet printing where often molten wax is used, be it in added manufacturing or in metal production processes or in extreme ultraviolet lithography (EUV) for the chip production where molten tin is used to generate the EUV radiation. For many of these industrial applications, a detailed understanding of the solidification process is essential. Here, by adopting a totally new optical technique in the context of freezing, namely TIR (Total-Internal-Reflection), we elucidate the freezing kinetics during the solidification of a droplet while it impacts on an undercooled surface. We show for the first time that at sufficiently high undercooling a peculiar freezing morphology exists that involves sequential advection of frozen fronts from the centre of the droplet to its boundaries. This phenomenon is examined by combining elements of classical nucleation theory to the large scale hydrodynamics on the droplet scale, bringing together two subfields which traditionally have been quite separated. Furthermore, we report a peculiar self-peeling phenomenon of a frozen splat that is driven by the existence of a transient crystalline state during solidification.