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Quasi-two-dimensional transition-metal dichalcogenides are a key platform forexploring emergent nanoscale phenomena arising from complex interactions.Access to the underlying degrees-of-freedom on their natural time scalesmotivates the use of advanced ultrafast probes sensitive to self-organisedatomic-scale patterns. Here, we report the first ultrafast investigation ofTaTe2, which exhibits unique charge and lattice trimer order characterised by atransition upon cooling from stripe-like chains into a $(3 \times 3)$superstructure of trimer clusters. Utilising MeV-scale ultrafast electrondiffraction, we capture the photo-induced TaTe2 structural dynamics -- exposinga rapid $\approx\!1.4$ ps melting of its low-temperature ordered state followedby recovery via thermalisation into a hot cluster superstructure.Density-functional calculations indicate that the initial quench is triggeredby intra-trimer Ta charge transfer which destabilises the clusters, unlikemelting of charge density waves in other TaX2 compounds. Our work paves the wayfor further exploration and ultimately rapid optical and electronicmanipulation of trimer superstructures.

Ultrafast optical melting of trimer superstructure in layered 1T'-TaTe2