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Ultrafast non-equilibrium dynamics offer a route to study the microscopicinteractions that govern macroscopic behavior. In particular, photo-inducedphase transitions (PIPTs) in solids provide a test case for how forces, and theresulting atomic motion along a reaction coordinate, originate from anon-equilibrium population of excited electronic states. Utilizing femtosecondphotoemission we obtain access to the transient electronic structure during anultrafast PIPT in a model system: indium nanowires on a silicon(111) surface.We uncover a detailed reaction pathway, allowing a direct comparison with thedynamics predicted by ab initio simulations. This further reveals the crucialrole played by localized photo-holes in shaping the potential energy landscape,and enables a combined momentum and real space description of PIPTs, includingthe ultrafast formation of chemical bonds.

Beyond the molecular movie: dynamics of bands and bonds during a photo-induced phase transition