arXiv · 1803.11022
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.
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Christopher W. Nicholson, Andreas Lücke, Wolf Gero Schmidt, Michele Puppin, Laurenz Rettig, Ralph Ernstorfer, Martin Wolf. 2018-03-29. Beyond the molecular movie: dynamics of bands and bonds during a photo-induced phase transition. https://doi.org/10.1126/science.aar4183
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