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