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Local Ionization Dynamics Traced by Photoassisted Scanning Tunneling Microscopy: A Theoretical Approach

Schüler M., Pavlyukh Y., and Berakdar J.

J. Phys. Chem. Letters 4, pp 1131 (2013)

For tracing the spatiotemporal evolution of electronic systems, we suggest and analyze theoretically a setup that exploits the excellent spatial resolution based on scanning tunneling microscopy techniques combined with the temporal resolution of femtosecond pump−probe photoelectron spectroscopy. As an example, we consider the laser-induced, local vibrational dynamics of a surface-adsorbed molecule. The photoelectrons released by a laser pulse can be collected by the scanning tip and utilized to access the spatiotemporal dynamics. Our proof-of-principle calculations are based on the solution of the time-dependent Schrödinger equation supported by the ab initio computation of the matrix elements determining the dynamics.

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