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 Schrodinger equation supported by the ab initio computation of the matrix elements determining the dynamics.

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

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 Schrooedinger equation supported by the ab initio computation of the matrix elements determining the dynamics.

Photoemission current imaging at the nanoscale is demonstrated by combining an atomic force microscope with laser excitation. Photoelectrons emitted from the sample are collected by the tip while the tip-sample distance is precisely controlled by their van der Waals force interaction. We observe pronounced photoemission current contrast with spatial resolution of 5 nm on a cesium covered Au(111) surface. This high spatial resolution can be attributed to the strong dependence of the local potential barrier on the tip-sample distance. Our experiments provide a method for photoelectron imaging with high spatial resolution and extend the functionality of state-of-the-art scanning probe techniques.

https://www-old.mpi-halle.mpg.de/mpi/publi/pdf/11147_13.pdf

Nanoscale imaging of photoelectrons using an atomic force microscope

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Nanoscale imaging of photoelectrons using an atomic force microscope