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Updated: May 5, 2026

Direct Imaging of Laser-driven Ultrafast Molecular Rotation
Published on: February 4, 2017
Vibronic motion with joint angstrom-femtosecond resolution observed through Fano progressions recorded within one
Joonhee Lee1, Shawn M Perdue, Alejandro Rodriguez Perez
1Department of Chemistry, University of California , Irvine, California 92697-2025, United States.
Abstract:
Electroluminescence (EL) in scanning tunneling microscopy (STM), which enables spectroscopy with submolecular spatial resolution, is shown to be due to radiative ionization with vibronic shape resonances that carry Fano line profiles. Since Fano progressions retain phase information, the spectra can be transformed to the time domain to reconstruct the vibronic motion. In effect, measurements within a molecule are accessible with joint space-time resolution at the Å-fs limit. We demonstrate this through EL-STM on the Jahn-Teller-active Zn-etioporphyrin radical anion and visualize the orbiting motion of scattered electrons upon sudden reduction and oxidation. We discuss the elements that enable spectroscopy with submolecular spatial resolution through EL-STM and the closely related STM-Raman process.
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