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Journal Article

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

MPS-Authors
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Nicholson,  Christopher
Physical Chemistry, Fritz Haber Institute, Max Planck Society;

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Puppin,  Michele
Physical Chemistry, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons104701

Rettig,  Laurenz
Physical Chemistry, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons21497

Ernstorfer,  Ralph
Physical Chemistry, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons22250

Wolf,  Martin
Physical Chemistry, Fritz Haber Institute, Max Planck Society;

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1803.11022.pdf
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Citation

Nicholson, C., Lücke, A., Schmidt, W. G., Puppin, M., Rettig, L., Ernstorfer, R., et al. (2018). Beyond the molecular movie: dynamics of bands and bonds during a photo-induced phase transition. Science, 362(6416), 821-825. doi:10.1126/science.aar4183.


Cite as: https://hdl.handle.net/21.11116/0000-0002-C619-3
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.