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

2018/03/31 by Christopher W. Nicholson, C. W. Nicholson, Andreas Lücke +11 · 2 citations
Engineering · Physics and Astronomy · #Nanowire Synthesis and Applications #Organic Electronics and Photovoltaics #Surface and Thin Film Phenomena #cond-mat.str-el

paper · pdf · doi:10.1126/science.aar4183

published as Nicholson et al. Science, Vol. 362, Issue 6416, pp. 821-825 (2018) · Main text and supplementary materials. Published in Science. This is the authors version of the work

openalex created_date 2018/04/06 · openalex publication_date 2018/11/15 · arxiv created 2018/11/16 · arxiv updated 2018/11/19 · openalex updated_date 2026/08/01

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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