期刊
ACS NANO
卷 8, 期 1, 页码 54-63出版社
AMER CHEMICAL SOC
DOI: 10.1021/nn405335h
关键词
scanning tunneling microscopy; submolecular spectroscopy; Jahn-Teller effect; electroluminescence; Fano line shape
类别
资金
- NSF Center for Chemical Innovation [CHE-082913]
- NSF graduate research fellowship [DGE-0808392]
- Direct For Mathematical & Physical Scien [0802913] Funding Source: National Science Foundation
- Division Of Chemistry [0802913] Funding Source: National Science Foundation
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 A-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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