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

TL;DR

This paper proposes a theoretical method combining scanning tunneling microscopy and femtosecond photoelectron spectroscopy to visualize local electronic and vibrational dynamics at surfaces with high spatial and temporal resolution.

Contribution

It introduces a novel theoretical framework for tracking local ionization dynamics using a combined microscopy and spectroscopy approach, supported by ab initio calculations.

Findings

Demonstrated the feasibility of using photoassisted STM to trace vibrational dynamics

Provided a theoretical model for spatiotemporal electronic evolution on surfaces

Showed potential for high-resolution dynamic surface analysis

Abstract

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.