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

Abstract

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

Main text and supplementary materials. Published in Science. This is the authors version of the work

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