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Two-dimensional melting is one of the most fascinating and poorly understoodphase transitions in nature. Theoretical investigations often point to atwo-step melting scenario involving unbinding of topological defects at twodistinct temperatures. Here we report on a novel melting transition of acharge-ordered K-Sn alloy monolayer on a silicon substrate. Melting starts withshort-range positional fluctuations in the K sublattice while maintaininglong-range order, followed by longer-range K diffusion over small domains, andultimately resulting in a molten sublattice. Concomitantly, the charge-order ofthe Sn host lattice collapses in a multi-step process with both displacive andorder-disorder transition characteristics. Our combined experimental andtheoretical analysis provides a rare insight into the atomistic processes of amulti-step melting transition of a two-dimensional materials system.

Coupled Sublattice Melting and Charge-Order Transition in Two Dimensions